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Synthesis and Characterization of Iron-Rich Glauconite Nanorods by a Facile Sonochemical Method for Instantaneous and Eco-friendly Elimination of Malachite Green Dye from Aquatic Environments
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Synthesis and Characterization of Iron-Rich Glauconite Nanorods by a Facile Sonochemical Method for Instantaneous and Eco-friendly Elimination of Malachite Green Dye from Aquatic Environments
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  • Aya Fadl Allah
    Aya Fadl Allah
    Materials Technologies and their Applications Lab, Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt
    Department of Chemistry, Faculty of Science, Beni-Suef University, Beni-Suef City 62514, Egypt
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  • Ahmed A. Abdel-Khalek
    Ahmed A. Abdel-Khalek
    Department of Chemistry, Faculty of Science, Beni-Suef University, Beni-Suef City 62514, Egypt
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  • Ahmed M. El-Sherbeeny
    Ahmed M. El-Sherbeeny
    Industrial Engineering Department, College of Engineering, King Saud University, P.O. Box 800, Riyadh 11421, Saudi Arabia
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    Orcidhttps://orcid.org/0000-0003-3559-6249
  • Wail Al Zoubi*
    Wail Al Zoubi
    Materials Electrochemistry Laboratory, School of Materials Science and Engineering, Yeungnam University, Gyeongsan 38541, Republic of Korea
    *Email: [email protected]
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    Orcidhttps://orcid.org/0000-0003-4213-8481
  • Mostafa R. Abukhadra*
    Mostafa R. Abukhadra
    Materials Technologies and their Applications Lab, Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt
    Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt
    *Email: [email protected]
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    Orcidhttps://orcid.org/0000-0001-5404-7996
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ACS Omega

Cite this: ACS Omega 2023, 8, 51, 49347–49361
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https://doi.org/10.1021/acsomega.3c07870
Published December 12, 2023

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Abstract

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Novel glauconite nanorods (GNRs) were synthesized by the sonication-induced chemical expansion and scrolling process of natural glauconite. The synthetic nanostructure was characterized by different analytical techniques as a superior adsorbent for the malachite green dye (MG). The synthetic GNRs were detected as porous nanorods with an average length of 150 nm to 5 μm, an average diameter of 25 to 200 nm, and a specific surface area of 123.7 m2/g. As an adsorbent for MG, the synthetic GNRs showed superior uptake capacity up to 1265.6 mg/g at the saturation stage, which is higher than most of the recently developed highly adsorbent dyes. The adsorption behavior and mechanistic properties were depicted by using modern and traditional equilibrium modeling. The kinetic assumption of the pseudo-first-order model (R2 > 0.94) and the classic isotherm of the Langmuir equilibrium model (R2 > 0.97) were used to describe the adsorption reactions. The steric investigation demonstrates that each active site on the surface of GNRs can adsorb up to three MG molecules (n = 2.19–2.48) in vertical orientation involving multimolecular mechanisms. Also, the determined active site density (577.89 mg/g) demonstrates the enrichment of the surface of GNRs with numerous adsorption receptors with strong affinity for the MG dye. The energetic study, including Gaussian energy (6.27–7.97 kJ/mol) and adsorption energy (9.45–10.43 kJ/mol), revealed that GNRs had physically adsorbed the dye, which might involve electrostatic attraction, hydrogen bonding, van der Waals forces, and dipole forces. The internal energy, enthalpy, and entropy determined the exothermic and spontaneous uptake of MG.

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1. Introduction

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In recent times, the accelerated growth of industries has resulted in significant environmental challenges, notably the issue of water pollution and its consequential impacts on both aquatic ecosystems and human health. (1,2) Various types of pollutants are discharged into the surroundings as a result of industrial operations, including dyes, pesticides, heavy metals, antibiotics, petrochemicals, and bacteria. (3,4) All of these aforementioned concerns possess substantial gravity, representing catastrophic challenges that pose a direct threat to the well-being of both human beings and all other forms of life. (5) Synthetic dyes are aromatic organic compounds that serve as crucial coloring agents for various sectors such as paper, plastic, leather, printing, and textiles. (6,7) Hence, it has been stated that an estimated quantity of over 7 × 105 tons annually of dyes manufactured is being discharged as contaminants into the natural environment and aquatic ecosystems. (8) The majority of synthetic dyes are known to possess toxicity and nondegradability, leading to a range of adverse consequences, including dermatitis, allergies, cancer, teratogenicity, skin irritation, carcinogenicity, and kidney damage. (8,9) Furthermore, the migration of dye molecules has adverse effects on the aquatic ecosystem, specifically impacting the photosynthetic activity and overall bioactivity of the species present. This pertains to the inhibitory effect of the dye surface on the penetration of sunlight into the deeper layers of water. (4,8) Malachite green (MG) is a frequently used dye, characterized as a synthetic organic molecule (C23H25ClN2) with a green hue. However, despite the widespread use of the MG dye in several industries, including the aquaculture, food, and pharmaceutical disinfection sectors, it has been recognized as a highly hazardous compound. (4,10,11) Insufficient treatment of MG results in a substantial release of this molecule into the aquatic environment, leading to a decrease in the oxygen levels in the water. Moreover, the presence of MG at high concentrations poses notable health risks, including mutagenesis, pulmonary toxicity, chromosomal fractures, tumor formation, and teratogenicity. (12,13)
Consequently, a variety of investigations have been accomplished to facilitate the advancement of technology aimed at the separation of MG from water supplies. Various technologies were utilized in this study, including adsorption, ion exchange, coagulation, biological oxidation, photocatalytic oxidation, nanofiltration, flocculation, and precipitation by chemicals. (7,14) Several considerations, including simplicity, effectiveness of elimination, recycling potential, environmental significance, and maintenance prices, impose significant limitations on the prospective implementation of the aforementioned procedures in a commercial and large-scale context. (15,16) The utilization of adsorption decolorization technologies has been suggested as a viable approach due to their affordability, accessibility, safety, cost-effectiveness, and recyclability, making them suitable for large-scale applications. (17,18) Hence, a variety of efficient natural and synthetic materials have been developed with the objective of eliminating synthetic dyes from water supplies. These materials have been evaluated based on factors such as the price of production, capacity to absorb dyes, accessibility to precursors, practicality for implementation, speed of adsorption, and recyclable properties. (16,19) The utilization of effective clay-based nanostructures has proven to be an effective technique for successfully eliminating both organic and inorganic chemicals, offering the benefits of cost-effectiveness and sustainability. (3,20) Most clay minerals have flexible multilayered aluminosilicate structures with significant ion exchange capacities, considerable chemical stability, a favorable reactive surface, an excellent adsorption capacity, and thermal resistance. (21−23)
In later periods, clay-based one-dimensional nanostructures (nanotubes) have been developed as an advanced modified form of clay with unique surface area and dispersion properties. (24,25) This occurred essentially by facile sonication-prompted chemical exfoliation followed by scrolling processes, which resulted in semicrystalline particles composed of scrolled single or several clay sheets that exhibit unique surface reactivity, surface area, porous structure, and adsorption capacities. (24,26,27) However, most of the studies introduced about the exfoliation and scrolling of the clay minerals focused on both kaolinite and bentonite; no previous studies have been introduced to investigate other clay minerals, such as glauconite. Glauconite is one of the common natural clay minerals that exhibits a potassium-ferric phyllosilicate structure (K, Na) (Fe3+Fe2+, Al, Mg)2(Si,Al)4O10(OH)2). Structurally, glauconite is composed of mixed layers of illite/smectite intercalated units, in which the alumina dioctahedral unit is between two units of silicon tetrahedron units containing interlayer K+ cations. (2829) Glauconite as a mineral shows significant natural reserves, low cost, metal-bearing chemical structure, attractive morphology, high surface area, promising catalytic properties, and high ion exchange capacity. (30,31) Therefore, the scrolling and exfoliation of glauconite into nanotubes will result in an innovative structure that exhibits unique physicochemical properties and adsorption capacity during the decontamination of different water pollutants. (32,33)
The introduced study involved the innovative synthesis of novel Fe-rich glauconite nanorod-like structures as superior adsorbents of malachite green dye with instantaneous removal efficiency. The evaluation of the adsorption characteristics was carried out using detailed studies, considering the main parameters and theoretical studies. The theoretical modeling involved the investigation of the classic models in addition to the advanced models to estimate the saturation adsorption capacity, active site density, number of adsorbed ions, adsorption energy, and thermodynamic functions.

2. Results and Discussion

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2.1. Characterization

2.1.1. XRD Analysis

The structural modifications as well as the dominant crystal phases were assessed based on the XRD patterns of the raw glauconite and synthetic GNRs, as well as the intermediate phases. The recognized pattern of raw glauconite significantly demonstrates the existence of glauconite as the dominant phase in addition to some impurities, which included quartz, calcite, feldspar, and hematite (Figure 1A). The identified glauconite form is represented by 1 M-glauconite poly type with a well-ordered crystalline structure of ISII ordered type and is characterized by a high K2O content and slight swelling properties. (34) The identification of glauconite has been established by analyzing XRD peaks previously stated (8.67, 19.72, 26.7, 34.78, 37.17, and 61.31°) with basal spacing of 10.18 Å (Figure 1A). (34−36) After the modification of the glauconite with DMSO, the obtained XRD pattern demonstrates significant deviation in the essential peaks of glauconite (8.01, 19.54, 26.5, 34.5, 36.8, and 61.1°) (Figure 1B).

Figure 1

Figure 1. XRD patterns of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), and synthetic glauconite nanorods (GNRs) (D).

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This validates the remarkable distortion in the structural units of glauconite after this step and the expected intercalation of the silicate layers with DMSO organic molecules. This was also signified by the detected increment in the basal spacing that expanded to 11.2 °C, demonstrating the swelling effect of the intercalated DMSO. The same observations were detected during the evaluation of the XRD pattern of methoxy glauconite (Figure 1C). The main peaks deviated to notable lower positions (7.47, 19.52, 26.5, 34.4, and 35.57°) (Figure 1C). This was also associated with a notable expansion effect on the silicate layers of glauconite, which appeared in the rise in the basal spacing to 11.81 Å. Regarding synthetic glauconite nanorods, the resulted pattern validates strong destruction of the structure units of glauconite and partial amorphization of its structure (Figure 1D). Most of the diffraction peaks of glauconite were reduced extensively, and the main peak around 2θ of 8° completely disappeared. Additionally, this observation confirms the notable occurrence of exfoliating and separating throughout the multilayered units, leading to the development of a novel semicrystalline form.

2.1.2. SEM and HRTEM Analysis

The changes in the morphological features during the production of the glauonite nanorods were followed based on the SEM (Figure 2) as well as the HRTEM (Figure 3) images. The starting glauconite shows the common massive and agglomerated form of glauconite with the commonly detected stacky and compact layers (Figure 2A). The intercalation of the layers with DMSO molecules caused notable exfoliation of the glauconite layers, which effectively separated from each other (Figure 2B). The exfoliation steps increased significantly after the incorporation of the methanol molecules, and the glauconite samples appeared as single layers overlaid each other (Figure 2C). During the initial stage of the scrolling steps and the incorporation of CTAB molecules, the separated glauconite layers exhibited slight binding and appeared in curvature form (Figure 2D). By the end of the scrolling and the modification steps in the existence of the sonication source, the sample reflects a complete change in the morphology to be in rodlike structures instead of the flaky form (Figure 2E,F). The obtained glauconite rodlike structure exhibits length within the range of 150 nm to 5 μm and diameter within the range of about 25 to 200 nm.

Figure 2

Figure 2. SEM images of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), CTAB intercalated glauconite (D), and synthetic GNRs (E and F).

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Figure 3

Figure 3. HRTEM images of raw glauconite (A), in-depth scrolled glauconite with lattice fingers structures (B and C), and the synthetic GNRs after extensive sonication treatment (D–F).

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The recognized HRTEM images of the assessed samples confirm the detected morphological anomalies, according to the SEM images (Figure 3). The glauconite platelets appeared as massive to nearly elliptic grains without marked internal properties (Figure 3A). The intercalated CTAB molecules made the glauconite grains peel off and start to roll; they turned into a multilayered, rodlike nanostructure with clear lattice finger structures (Figure 3B,C). The extensive scrolling process, especially under the sonication effect, causes a significant condensation effect on the formed rod structure, which is in a smooth cylindrical form, suggesting separated scrolling of each layer into a single rod (Figure 3D–F). Therefore, there are no indications or observations of the previously reported lattice finger structures. However, the focus images on the surface of the finally obtained rods reflected their highly porous properties, which give the structure ribbonlike morphologies and properties, (Figure 3F). Such morphological features are associated with an increase in the surface area of the structure and its porosity, which induces its qualification to be applied as effective adsorbents for different species of dissolved water pollutants.

2.1.3. FTIR Analysis

The changes in the main chemical functionals during the synthesis steps were followed based on the observed FTIR spectra of the raw glauconite and synthetic GNRs in addition to the intermediate structures (Figure 4; Table 1). Regarding the raw glauconite, the obtained spectrum clearly displays its widely reported composition as a clay mineral with an aluminosilicate structure. These involved the identification of the corresponding bands of Si–O–Si, Fe–OH, Si–O, Si–O–Fe, Si(Al)–O-Si, and OH groups (Figure 4; Table 1). The detected hydroxyl groups around 3500 cm–1 were assigned to either the adsorbed water or the metal hydroxides with the glauconite structure. (37) However, the identified hydroxyl groups corresponding to the absorption band around 1600 cm–1 signify the interlayer free water molecules (38) (Figure 4; Table 1). Moreover, the recognized bands around 800 and 490 cm–1 display the enrichment of the glauconite with iron, which is in agreement with its XRF chemical analysis. Regarding the investigated spectra of both DMSO intercalated glauconite and methoxy glauconite, they show similar bands of raw glauconite with no detectable bands related to their organic structures (Figure 4; Table 1). There is only a slight fluctuation in the exact locations of the primary basic groups’ matching bands, which might validate the structural effect of the intercalated organic molecules of DMSO and methanol on the structural units of glauconite (Figure 4; Table 1). Moreover, there is slight splitting for the identification band of Si(Al)–O-Si around 1000 cm–1. This validates the distortion of the glauconite structural units (octahedron and tetrahedron units) as a result of the partial swelling and exfoliation of silicate layers. (39) After the formation of GNRs, the absorption bands of the main structural units of glauconite deviated at a high rate. Moreover, the splitting of the identification band of Si(Al)–O-Si around 1000 cm–1 increased to a considerable degree, validating an increment in distortion and exfoliation degree (Figure 4; Table 1). Moreover, new bands were detected at 1475, 2850, and 2919 cm–1 that strongly signify the organic structure of the CTAB molecules that were used during the exfoliation and scrolling processes (Figure 4; Table 1)

Figure 4

Figure 4. FTIR spectra of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), and synthetic GNRs (D).

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Table 1. FTIR Detectable Bands of Glauconite during the Various Alteration Procedures and the Corresponding Chemical Groups
absorption bands (cm–1)functional chemical groups
glauconiteDMSO/glauconitemethoxy glauconiteGNRs
3532342035303535stretching and bending vibrations of −OH groups (40)
   2919asymmetric stretching vibrations of −CH2 (32)
   2850symmetric stretching vibrations of −CH2 (32)
1639163516391638interlayer water molecules (38)
   1475excited methylene group (41)
1020102210241019Si(Al)–O–Si asymmetric stretching (3,37)
804806805810Fe23+ OH/Fe2+Fe3+OH bending (37)
681680681679bending vibration of Si–O and/or −OH (37)
493495.6492495.2Si–O–Fe3+ (40,42)
445.6445.02444443Si–O–Si (40,42)
The previously reported chemical findings of GNRs based on the FTIR analysis are in agreement with the recognized elemental contents determined relying upon EDX spectra (Figure 5). The essential elements of the silicate structures were detected clearly, such as O, Si, Fe, and K (Figure 5). The significant increase in the Fe content after the scrolling process of glauconite into GNRs reflected the strong diffusion of the structural ion element or iron oxide impurities during exfoliation and extensive destruction of the glauconite silicate units.

Figure 5

Figure 5. EDX spectrum of the synthetic GNRs and the corresponding elemental composition.

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2.1.4. Textural Analysis

The textural properties of the synthetic GNRs were assessed in terms of porosity and surface area properties based on the obtained N2 adsorption/desorption isotherm curve (Figure 6). The observed curve displays the IV isotherm type with a notable hysteresis loop of H3 type (Figure 6). This validates the nanoporous (mesoporous) properties of the synthetic GNRs, which are associated essentially with the evacuation and/or filling of tabular or cylindrical nanopores via capillary condensation mechanisms. (32,43) The measured surface area of GNRs is 123.7 m2/g, which is a significantly promising value during the assessment of the product either as an ornamental or as a heterogeneous catalyst. Regarding the pore size distribution properties, the GNR particles' exhibit pore size ranges from 1.5 to 10 nm with an average pore diameter of 4.16 nm, which confirms the mesoporous structure.

Figure 6

Figure 6. Plotted nitrogen adsorption/desorption isotherm curve of the synthetic GNR particles and the pore size distribution properties.

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2.2. Adsorption Results

2.2.1. Influence of pH

From pH 2 to 8, the effect of the aquatic solutions’ pH on the adsorption properties of GNRs as prospective MG dye adsorbents was examined experimentally. All of these experiments were done after meticulously adjusting all of the influencing factors to set levels (MG concentration: 100 mg/L; volume: 100 mL; time: 120 min; solid dosage: 0.2 g/L; temperature: 20 °C). Based on the amounts of MG adsorbed using GNRs, there was a clear improvement when the pH of the polluted solutions tested went from 2 (20.6 mg/g) to 8 (140.8 mg/g) (Figure 7). GNRs have the ability to operate as particularly successful adsorbents throughout the real treatment efforts in line with the US EPA’s established pH limit for industrial effluents (pH 6 to 9) along with the laboratory-tested performances of GNRs at varying pH levels. (44) The investigation of the combined ionizing traits of MG dye plus the prevailing surface charges across the frameworks of GNRs may be utilized to illustrate the verified improvement in the determined adsorption behavior.

Figure 7

Figure 7. Influence of the solution pH on the uptake of MG dye by GNRs.

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According to the pH-dependent ionization properties of MG dye, it has a pKa value of 10.3, and it is in a stable protonated state at pH levels below this value and in a deprotonated state at pH levels above this value. (45,46) In highly acidic conditions (pH 2.0), the protonated forms (MGH+) can be made, but in alkaline conditions, the colorless carbinol basic species can be found. (46,47) As a result, the common color of the evaluated MG dye remains stable from pH 3 toward pH 7, after which it declines dramatically with increasing solution pH upward of 11. Therefore, it is recommended to evaluate the adsorption studies in a controlled range between acidic and neutral situations. (7,45) In terms of MG ionization characteristics, its charged ions possess strong electrostatic repellence with already-existing positively energized fundamental groups of GNRs at low pH levels (acidic circumstances). The continual generation of hydroxyl anions while raising the pH of the evaluated solutions is coupled with substantial deprotonation influences on the GNRs' active groups, which are negatively charged within this pH range. As a result, the positively charged MG species are electrostatically captured in significant quantities. (43,48,49)

2.2.2. Kinetic Assessment

2.2.2.1. Influence of Duration
The influence of the adsorbing period on the attained decolorization opportunities of MG by GNRs was investigated in a controlled investigation. The adsorption duration was varied within the range of 30–1320 min while keeping the levels of the primary influencing variables constant. These factors included the concentration of MG (100 mg/L), quantity of GNRs (0.2 g/L), volume of the solution (200 mL), temperature (20 °C), and pH (7). The decolorization properties of GNRs as potential adsorbents for MG demonstrate significant enhancements in both adsorption rates and capacities in mg/g, as well as the ability to extend the duration of the testing period in a regulated manner (Figure 8A). The effects of this enhancement may become significantly noticeable after 840 min. Subsequently, the extended period of the trials does not exhibit any significant impact on the rates of adsorption or the quantities of retained MG, indicating a state of stabilization or equilibrium conditions (Figure 8A). The particulates of GNRs in this specific form exhibit a certain degree of equilibrium MG dye absorption capacity at 241.3 mg/g (Figure 8A). The significant increase in the adsorption of MG and its quick rates are due to the existence of lots of unoccupied active positions on the GNR particles at the first stages of the decolorization events. (32) As the duration of testing increases, there is a progressive increase in the adsorption of MG into the unoccupied sites of GNRs. Consequently, the occupation and the increased fill of these vacant sites result in a substantial decrease in their accessibility. Therefore, there was a notable decline in the actual rates of adsorption during a certain time frame, and the GNRs demonstrated noteworthy enhancements in their adsorption properties that were overlooked. After exhaustively consuming all of the preexisting sites with the MG, researchers have successfully determined the equilibrium state of GNRs. (3)

Figure 8

Figure 8. Influence of contact time on the uptake of MG by GNRs (A), intraparticle diffusion curve during the uptake of MG (B), fitting of the MG uptake data with the common kinetic models (C), influence of MG starting concentrations on the uptake capacities of GNRs (D), fitting of the MG uptake data with the classic Langmuir model (E), fitting of the MG uptake data with the classic Freundlich model (F), fitting of the MG uptake data with the classic D–R model (G), and fitting of the MG uptake data with the advanced monolayer equilibrium model of one site of energy (H).

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2.2.2.2. Intraparticle Diffusion Behavior
The adsorption operations of MG utilizing GNRs exhibit an intraparticle diffusion trend demonstrating segmented characteristics consisting of three clear discrete trends that do not connect with the beginning points (Figure 8B). This finding demonstrates that the uptake of MG involves collaborative mechanisms, along with the important role that MG ion diffusion plays in the pathway of the functional sites of GNRs. (41,50) The process can involve three main mechanisms: (A) adsorption onto active sites located on the external surface, (B) diffusion within the particle, and (C) the influence of the saturation or equilibrium phase. (51) The initial phase of the experiment suggests that the external adsorption processes of MG were operational at the beginning of the testing. The efficacy of this stage is contingent upon the overall quantity of surface-active receptors (Figure 8B). (17) A subsequent phase has been discovered through the extension of time (Figure 8B), which signifies the implementation of extra mechanisms such as the influence of MG transportation operations and layered adsorption interactions. (21,51) The prevailing stage in which GNRs exist in an equilibrium state for MG adsorption has been conclusively determined. This observation provides evidence that the MG ions that were caught have entirely filled the effective receptors (Figure 8B). (16,41) The regulation of MG elimination activities during this stage is governed by a range of processes, which may involve molecular interactions and/or mechanisms such as interionic attractions. (52)
2.2.2.3. Kinetic Behaviors
The kinetic properties of the MG uptake operations by GNRs were demonstrated using the existing kinetic theories of the pseudo-first-order (P.F.) and pseudo-second-order (P.S.) models. The degree of agreement between the kinetic assumptions of the two analyzed models and our findings of MG uptake has been assessed employing standard nonlinear fitting criteria. These levels were determined based on both correlation coefficients (R2) as well as chi-squared (χ2) values. The results of this assessment can be found in Table 2 and are visually shown in Figure 8C. The obtained R2 values and χ2 findings suggest that the characteristics and fundamental principles of the P.F. offer a more accurate representation of the MG adsorption processes by GNRs in comparison with the evaluated P.S. model. The observed agreement between the laboratory-determined capacity of GNRs at the point of equilibrium (240 mg/g) and the value predicted through theoretical approaches (254.8 mg/g) supports these findings (Table 2). The primary mechanism responsible for the sequestration of MG by GNRs, as per the principles of the P.F. model, can be attributed to physical events. These processes may involve significant contributions of van der Waals forces in addition to electrostatic attractions, as suggested by earlier investigations. (53,54) Although the equation proposed by the P.F. model for eliminating MG by GNRs is more appropriate compared with the equation offered by the P.S. theory, the uptake behaviors nevertheless exhibit substantial agreement with the kinetics of the P.S. theory. As a result, it was supposed that further frequent weakly operated chemical processes, among which are hydrogen binding, formation of complexes, and sharing of electrons, could have a secondary role or have a minimal effect on the processes. (41,53) The creation of a chemically captured MG layer was subsequently followed by the formation of a physically captured layer, employing the first chemically retained layer as the base. (55)
Table 2. Mathematical Parameters of the Addressed Kinetic Models
kinetic models
modelparameters293 K
pseudo-first-orderK1 (1/min)0.0042
Qe(Cal)(mg/g)254.8
R20.94
X23.95
pseudo-second-orderk2(mg/g min)1.049 × 10–5
Qe(Cal)(mg/g)330.2
R20.90
X26.23

2.2.3. Equilibrium Investigation

2.2.3.1. MG Concentrations
The adsorption behaviors of GNRs were investigated by varying the initial concentration of the target molecules, MG, within a range of 100 to 700 mg/L. To ensure accuracy, all relevant factors, including period (24 h), tested volume (100 mL), incorporated solid dosage (0.2 g/L), and operating temperature (293–313 K), were carefully controlled and adjusted to certain values. In the evaluation of the adsorbing aspects of GNRs, the initial concentration serves as a significant variable in elucidating equilibrium aspects and maximum capacities (Figure 8D). Upon conducting an analysis of the properties of GNRs under the influence of elevated concentrations of MG ions, a significant increase in the quantity of MG adsorption was observed (Figure 8D). The existence of increased levels of MG within certain volumes induces a significant enhancement in the migration, mobility, and driving forces of the dye ions. Consequently, this leads to increased collisions as well as chemical interactions via the binding sites located on the external surface of GNRs, thereby improving the efficiency of uptake. (41,52) The increase in the quantities of MG adsorbed in relation to the initial levels under investigation may be observed distinctly up to certain values that were evaluated (Figure 8D). Subsequently, an increase in the starting level of MG has been perceived to have a significant impact on the adsorbed quantities of MG molecules by GNRs. This effect, which has been previously overlooked, plays a crucial role in determining the equilibrium state and achieving the most favorable adsorption conditions. The equilibrium state of GNRs as adsorbents may be observed at various temperatures (293, 303, and 313 K) after being subjected to a concentration of 500 mg/L of MG. The exact performances of the GNRs for adsorbing MG are measured to be 1156, 985.1, and 890.2 mg/g at the respective temperatures (Figure 8D). The diminution in the adsorption of MG via GNRs that can be observed in the context of the experiment’s temperature suggests that the processes were exothermic.
2.2.3.2. Giles’s Classification
The MG equilibrium graphs were categorized using GNRs according to the criteria established by Giles’s classification. The analysis showed that these curves exhibited an L-type equilibrium behavior, as depicted in Figure 8D. (56) The equilibrium aspects of the L-type play a crucial role in the profound effects resulting from intermolecular attraction forces during the adsorption stages of MG via GNR particulates. These effects are further amplified by the intense interactions between MG molecules and the framework of GNR particulates that is highly reactive. (57) Based on the properties of the L-type isotherm, it was possible that a complete formation of an adsorbed MG monolayer would occur on the exterior interfaces of GNR particles. (58) Moreover, the observed isothermal activity implies that the GNR nanostructures have been improved by the incorporation of a variety of activated and empty uptake sites. These receptors demonstrate significant selectivity toward the target molecules, specifically the MG compounds, during the adsorption process, especially when the initial levels are low.
2.2.3.3. Conventional Isotherms
The equilibrium assessments of the MG elimination pathways by GNRs nanoparticles were investigated by using the key principles of the traditional Langmuir, Freundlich, and Dubinin–Radushkevich (D–R) hypotheses. Nonlinear regression modeling was used to evaluate the congruence that exists between the isotherm assumptions of various models and measured findings, employing illustrative mathematical equations. The assessment relied on the determination coefficient (R2) alongside the chi-squared (χ2) statistic. The assessment is displayed in Table 3 and depicted in Figures 8E–G. The results obtained from the analysis of R2 and χ2 that indicate that the MG retained actions via the GNR nanostructures align more closely with the basic concepts of the Langmuir isotherm (Figure 8E; Table 3) instead of the fundamental properties of the Freundlich isotherms (Figure 8F; Table 3). The Langmuir equation depicts the uniform distribution of MG adsorption onto GNR nanoparticles, specifically targeting the empty and active sites and forming a monolayer arrangement. (53,54) Further, it has been observed that the calculated RL value of the MG adsorption actions facilitated by the GNR nanostructures is below 1. This suggests that the reactions exhibit desirable characteristics, as indicated by previous studies. (16,17) The anticipated maximum absorption capacities (Qemax) of GNRs at different temperatures are as follows: 1266.8 mg/g at 293 K, 1052.42 mg/g at 303 K, and 942.63 mg/g at 313 K, as indicated in Table 3.
Table 3. Statistical Parameters of the Conventional and Modern Isotherm Models
conventional isotherm
  293 K303 K313 K
Langmuir modelQmax(mg/g)1266.81052.42942.63
b (L/mg)3.35 × 10–51.03 × 10–57.09 × 10–6
R20.9760.9880.991
X23.291.661.02
Freundlich model1/n0.7090.6230.598
kF(mg/g)125.09320.9447.6
R20.9320.9700.976
X25.392.222.34
D–R modelβ (mol2/kJ2)0.007870.008660.0127
Qm(mg/g)1162.31006.8912.8
R20.9120.960.971
X27.313.643.02
E (kJ/mol)7.977.596.27
Advanced isotherm
monolayer model of one energyR20.9820.9880.992
X21.741.0890.428
n2.192.412.48
Nm (mg/g)577.89435.38379.39
QSat (mg/g)1265.61049.2940.8
ΔE (kJ/mol)–9.45–9.97–10.43
The fundamental concepts of the D–R model’s isotherm, as depicted in Figure 8G, elucidate the energy variations of GNRs nanomaterials while they undergo the process of capturing the MG dye. These energy variations remain unaffected by the surface features of the particles, which can either be heterogeneous or homogeneous. (59) The theoretically defined parameter known as Gaussian energy (E), determined from the D–R assessment approach, plays a crucial role in determining the sort of MG uptake mechanisms that are affecting it, i.e., whether they are chemical pathways or physical behaviors. Processes characterized by energies (E's) of below 8 kJ/mol, spanning from 8 to 16 kJ/mol, and over 16 kJ/mol are suggestive of distinguishable physical, poor chemical to complex (physical and weak chemical), and forceful chemical specifications, respectively. (16,59) The obtained E values using GNRs were verified to fall inside the allowed energy limits of physical activities (<8 kJ/mol) (Table 3).
2.2.3.4. Advanced Isotherm Modeling
The investigation of advanced equilibrium models that are in accordance with the principles of statistical physics concepts can yield valuable insights into specific features of adsorption operations, particularly in terms of the interfaces between the adsorbent and adsorbate as well as the exterior properties of the solid particles involved. The numerical parameters obtained from these models, including the energetic and steric elements, have the opportunity to be used to highlight the mechanistic processes. The steric components included three key parameters: the quantity of functionally active sites on GNRs filled with the target molecule of MG (Nm(MG)), the total amount of MG molecules captured by every site (n(MG)), and the maximum absorption capacity of GNRs under a saturated state (Qsat). The energetic parameters considered in this study were the energy required for MG elimination (ΔE), the internal energy (Eint), the free enthalpy (ΔG), and the entropy (Sa). A computational model of MG uptake processes has been conducted using nonlinear fits and the illustrated equations corresponding to these models. The achievement of this task was facilitated by the use of multivariable nonlinear regression simulations in conjunction with the Levenberg–Marquardt iterating approach. The MG adsorption procedures by GNRs were shown using a monolayer model that had a single energy site (Table 3; Figure 8H).
Steric Parameters
Number of Retained MG (n) at a Single Site
The numerical results of the n(MG) factor strongly indicate the manner in which the MG ions have been adsorbed on the outermost layers of the GNRs, either vertically or horizontally. Additionally, these values provide insights into the mechanistic pathways involved, namely, if there are multidocking processes or multi-interaction mechanisms occurring. The procedures most affected by multidocking pathways involve the acquisition of many MG molecules through the binding of several uptake receptors in horizontal arrangements. The retention mechanisms of the ions with a value of less than 1 are linked to the horizontal configuration of the ions that are bonded. On the other hand, systems exhibiting values greater than 1 exhibit both nonparallel and vertical alignment for the retained MG. The observed uptake operations in these systems are predominantly regulated by multi-ionic pathways that entail the binding of numerous dyes into a single site. (16,60) The observed levels of n(MG) all over the process of MG capture by GNRs (with a range of n values between 2.19 and 2.48) exhibit values that surpass 1, as depicted in Figure 9A and Table 3. Consequently, the MG molecules were adsorbed through multi-ionic mechanistic steps, wherein each adsorption site of the GNRs had the capacity to accommodate up to three ions and exhibited a vertical orientation with nonparallel characteristics. In the context of temperature implications, the calculated values of n(MG) for GNRs provide confirmation that they are pertaining to the temperature rise from 293 to 313 K (Figure 9A). The observed phenomenon of increased aggregation aspects of the MG immediately following its adsorption onto GNRs at higher temperatures has frequently been ascribed to this factor. (61) Furthermore, the aforementioned observation serves as evidence for the existence of thermal activation actions that occur prior to the capture of MG by GNRs. (2,62,63)

Figure 9

Figure 9. Variations in the quantity of MG molecules retained per site over the surface of GNRs (A), variations in the density of active sites with regard to temperature (B), fluctuations in the predicted uptake capacity of MG during the point of saturation of GNRs (C), shifts in entropy values in relation to MG concentration as well as temperature (D), variations in internal energy values with respect to MG concentration alongside temperature (E), and variations in enthalpy values as a function of MG concentration alongside temperature (F).

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Occupied Receptor Density (Nm)
The density of MG-filled receptors (Nm) on GNRs is a significant indicator of the overall number of available and effective retention sites on the surfaces of the nanoparticles involved in the chemical reaction (Figure 9B and Table 3). The predicted Nm(MG) values of GNRs at different temperatures, specifically 577.89 mg/g (293 K), 435.4 mg/g (303 K), and 379.4 mg/g (313 K), exhibit considerable promise when compared to previous research on clay minerals in general and their transformed frameworks. The Nm(MG) values of GNRs exhibit temperature-dependent irreversible relationships (Figure 9B; Table 3). The measured values of n(MG) align with this finding, as an increase in aggregation affinities leads to a decrease in the total number of filled sites. Additionally, the temperature has an impact on the dominant condition of the sites that are filled. (2,64) The application of high-temperature conditions has been found to have a positive impact on the activation of uptake sites for GNRs. This effect can be attributed to the exposure of further active sites as well as the presence of new energetic site groups. (64,65) There is a direct relationship between the increase in adsorption temperature and the decrease in the viscosity level of the MG solutions. (66) Consequently, the mobility and diffusion activity of water-soluble MG molecules exhibit a significant increase upon interaction with additional reactive sites.
Saturation Adsorption Properties (Qsat)
The saturation level of the MG sequestered effectiveness of GNRs, denoted as Qsat, represents the most reliable estimate for the maximum quantity of MG that can be adsorbed. The amounts of Qsat are impacted by two main factors, which are the total quantity of retained MG molecules per site (n(MG)) along with the formerly calculated densities of the filled sites (Nm(MG)). GNRs exhibit significant potential as a highly effective adsorbent for the adsorption of MG. The Qsat (saturated adsorption capacities) values of GNRs at various temperatures have been calculated to be 1265.6 mg/g at 293 K, 1049.2 mg/g at 303 K, and 940.8 mg/g at 313 K. The exothermic characteristics of the MG-capturing activities by GNRs are affected by the adverse impact of temperature (Figure 9C; Table 3). Additionally, this finding suggests that the impact of the temperature at which the adsorption process occurs on thermal collisions is increasing, resulting in a decline in the effectiveness of MG sequestration. (60) Furthermore, the observed characteristics of Qsat, which are driven by temperature adsorption, are consistent with the previously established patterns of Nm(MG) instead of n(MG). This suggests that the effectiveness of adsorption is impacted by the abundance of vacant sites in contrast to every active site’s distinctive capacity.
Energetic Assessment
Uptake Energy
The energy changes (ΔE's) associated with the uptake processes of MG exhibit regular patterns that may be attributed to either chemical or physical triggers. The physical processes that exert influence exhibit energy levels below 40 kJ/mol, but the chemical pathways possess levels of energy over 80 kJ/mol. The categorization of physically occurring mechanistic activities is dependent on adsorption energy levels. The aforementioned interactions encompass coordination exchanges (40 kJ/mol), forces of dipole bonding (2–29 kJ/mol), hydrogen bonds (<30 kJ/mol), van der Waals forces (4–10 kJ/mol), and hydrophobic bonds (5 kJ/mol). (61,64) The computational estimation of the uptake energy by MG (ΔE) was performed using eq 1, which incorporates the solubility factors of MG in water (S), the gas constant (R = 0.008314 kJ/mol·K), the MG level during the half-saturating state of GNRs, and the absolute temperature (T). (65)
ΔE=RTln(SC)
(1)
The energy estimations for MG capture by GNRs fall inside the range of −9.45 to −10.43 kJ/mol, as seen in Table 3. Hence, the primary mechanisms behind the absorption of MG by GNRs may be attributed to physical phenomena, particularly van der Waals forces (ranging from 4 to 10 kJ/mol), dipole bonding forces (ranging from 2 to 29 kJ/mol), and hydrogen binding forces (below 30 kJ/mol). Moreover, the observed negative signs of ΔE throughout the sequestration of MG by GNRs are consistent with formerly described experimental findings, indicating that the underlying mechanisms are exothermic.
Thermodynamic Investigations
Entropy (Sa)
The Sa properties of the MG sequestration operations by GNRs effectively demonstrate the characteristics of order and disorder on the exterior surfaces of these particles when exposed to different levels of dye ions as well as the specified reaction temperature. The properties of Sa have been examined based on the results obtained from eq 2, employing the aforementioned documented values for Nm(MG) and n(MG), together with the expected level of MG after the half-saturation phase of GNRs (C1/2).
SaKB=Nm{ln(1+(CC12)n)−n(CC12)nln(CC12)1+(CC12)n}
(2)
Based on the obtained data, it can be noted that the entropy levels (Sa's) exhibit a notable decrease throughout the process of MG adsorption by GNRs, particularly in the experiments conducted with very high concentrations of MG (Figure 9D). The observed trend demonstrates a significant reduction in the disorder features of the interfaces of GNR particulates as the levels of MG rise. Furthermore, the entropy functions further support the effective docking of the MG inside the existing inactive and unbound interaction receptors of the GNRs in the context of slightly lower concentrations of the dye molecules. (61,65) The experimental results shown in Figure 9D indicate that the maximum entropy values were seen when MG was captured by GNRs at equilibrium concentrations of 116.9 (at a temperature of 293 K), 111.5 (at a temperature of 303 K), and 102.8 mg/L (at a temperature of 313 K). The equilibrium levels of MG observed in this study exhibit a notable resemblance to the expected values for GNRs during their half-saturation phases. Consequently, the surplus of MG ions is unable to bind to the unoccupied locations of GNRs. Furthermore, the conspicuous reductions in the reported entropy suggest a noteworthy decrease in the quantity of accessible sites accompanied by a major loss in the degrees of freedom and diffusion characteristics of the MG ions. (66,67)
Internal Energy and Free Enthalpy Characteristics
The present study assessed the internal energy (Eint) associated with the sequestration of MG via GNRs as well as the changes in free enthalpy (G) resulting from variances in dye concentration as well as operational temperature. These evaluations were conducted using values obtained from eqs 3 and 4, which were computed using previously established parameters including Nm(MG), n(MG), C1/2, and the translation partition (Zv). (65)
EintKBT=nNm[((CC1/2)nln(CZv)1+(CC1/2)n)−(nln(CC1/2)(CC1/2)n1+(CC1/2)n)]
(3)
GKBT=nNmln(CZv)1+(C1/2C)n
(4)
The calculated internal energy (Eint) values for the MG sequestration activities by GNRs possess negative signals. Notably, these findings demonstrate a significant decrease as long as the temperature increases from 293 to 303 K (Figure 9E). This finding adds further evidence to the exothermic along with intrinsically spontaneous character of the MG removal mechanisms by GNRs. Consistent patterns of reactions and characteristics have been noticed in connection with the predetermined levels of Sa. The G values are characterized by negative signals and demonstrate a reversible dependence on the sequestration temperature under the test. This supports the spontaneity and exothermic character of the MG retention by GNRs and points to a decline in the feasibility characteristics (Figure 9F).

2.2.4. Recyclability

The investigation of the possibility of GNRs as a reusable adsorbent for the efficient elimination of MG dye has been conducted considering its significance in the assessment of the product for commercial and practical uses. The GNR nanoparticles utilized in the study underwent an intensive rinsing procedure using distilled water for a duration of 10 min, which was repeated five times. The purified GNRs were afterward subjected to a drying process at a temperature of 60 °C for a duration of 8 h. This was done to prepare them for further use in additional cycles of MG adsorption. The conducted recyclability studies were performed while considering the variables of adsorption under a pH of 8, a dose of 0.20 g/L for GNRs, a concentration of 100 mg/L for MG, an interval of 24 h, an overall volume of 100 mL, and a temperature of 293 K. Based on the six cycles conducted to assess the recycling potential, the use of GNRs as the adsorbent demonstrates significant stability and exceptional qualities for recyclability, as shown by the achieved efficacy of MG adsorption (Figure 10). The recyclable properties of GNRs resulted in varying levels of adsorption performance throughout the six rounds. The adsorption performance values were 241.3 mg/g (cycle 1), 238.7 mg/g (cycle 2), 230.2 mg/g (cycle 3), 218.4 mg/g (cycle 4), 200.7 mg/g (cycle 5), and 178.5 mg/g (cycle 6) (Figure 10). The repeated recycling of GNRs leads to slight decreases in the observed adsorption capabilities of MG. The observed behavior could possibly be attributed to the anticipated reduction in the quantity of GNR nanoparticles throughout the washing steps or the ongoing formation of complexes between the chemical structure of the MG molecule and the structural framework of the GNRs.

Figure 10

Figure 10. Recyclability properties of the synthetic GNRs during the uptake of MG dye.

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2.2.5. Comparison Study

The calculated capacity of the GNR adsorbent has been compared to other explored adsorbents in the literature (Table S3). The results reveal that GNRs have a higher capacity than the other materials, which include clay-based adsorbents, graphene oxide/Fe3O4 composites, nZVI/BC composite, Sr5xBa3x(PO4)3(OH)/Fe3O4, mesoporous carbon, sulfonated coal, magnesium hydroxyapatite, activated carbon, activated carbon, hydroxyl functionalized coal, chitosan/poly(acrylic acid)/bentonite, and halloysite nanotubes (Table 4). This supports the significance of the produced structure as an improved adsorbent with high adsorption performance, simple synthesis approaches, excellent recyclability, cheap cost, and readily available precursors.
Table 4. Comparison between the MG Uptake Capacity of GNRs and Other Studied Adsorbents in the Literature
adsorbentsQmax (mg/g)references
activated carbon395 (68)
chitosan/poly(acrylic acid)/bentonite454.5 (69)
nZVI/BC composite515.77 (11)
MAL456.62 (70)
rGO476.2 (71)
SS.C (Qmax)454.34 (4)
FHAP-SH625 (72)
Artocarpus odoratissimus leaves422 (73)
Sr5xBa3x(PO4)3(OH)/Fe3O4526 (47)
Fe3O4/PT/GO560.5 (74)
Mg.HPANFs (Qmax)710.93 (7)
hydroxyl functionalized coal763 (19)
mesoporous carbon476.1 (75)
GNRs1265.6this study

3. Conclusions

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A novel nanostructure of glauconite nanorods (GNRs) was synthesized effectively with an average diameter of 25–200 nm, an average length of 150 nm–5 μm, a BET surface area of 123.7 m2/g, and an average pore diameter of 4.16 nm. The formation of GNRs as mesoporous nanostructures was confirmed by different analytic techniques, including XRD, SEM, HRTEM, and BET. As an adsorbent of MG dye, it displays a strong adsorption capacity (1265.6 mg/g) compared to numerous studied adsorbents. This was assigned to its high surface area, high surface reactivity, and significant existence of numerous active sites (active site density = 577.89 mg/g). Monolayer and homogeneous uptake of MG on the surface of GNRs was concluded depending on the adsorption’s strong match with the Langmuir theory. Moreover, the number of adsorbed MG ions per site (n > 1) depicts how the adsorbed ions are oriented vertically by multimolecular mechanistic pathway. According to the energetic study (Gaussian energy (6.27–7.97 kJ/mol) alongside uptake energy (9.45–10.43 kJ/mol) together with the thermodynamic characteristics, MG sequestration by GNRs has taken place spontaneously via exothermic and physical processes.

4. Experimental Work

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4.1. Materials

The natural glauconite mineral was obtained from the El-Gedida area, El-Bahariya Oasis, Western Desert, Egypt. The studied sample displayed a chemical composition that consisted of SiO2 (52.2%), Fe2O3 (23.14%), K2O (6.48%), Al2O3 (6.12%), MgO (3.53%), CaO (0.27%), SO3 (0.17%), P2O5 (0.10%), Na2O (0.08%), TiO2 (0.11%), MnO (0.01%), and 7.8% L.O.I. Cetyltrimethylammonium bromide (CTAB) (>98%), dimethyl sulfoxide (DMSO) (>99.5%), NaOH (97%), and methanol (>99.9%) were acquired from Sigma-Aldrich, Egypt, and were used in the glauconite transformation process.

4.2. Synthesis of Glauconite Nanorods (GNRs)

The synthesis of the glauconite nanorods was produced according to the reported scrolling procedures by Abukhadra et al. (32) About 40 g of the starting glauconite mineral, after extensive grounding, was dispersed in 200 mL of diluted DMSO solution (80% DMSO/10% water) under vigorous stirring for 72 h. This particular procedure is of the greatest significance in the process of breaking the intermolecular bonds present within the layers of clay, especially the illite units of the glauconite structure. After that, the formed product was washed by methanol for five runs, and each washing run continued for about 20 min, forming methoxy glauconite (MX/G) with organophilic properties. The obtained MX/G fractions were immersed in aqueous solutions of CTAB as an expansion reagent (60 g in 200 mL) at room temperature under continuous stirring for 48 h at 1000 rpm to achieve successful exfoliation of the glauconite sheets. After that, the system was treated by sonication waves for 96 h in the presence of a sonication source of 240 W power supply to guarantee the rolling of the exfoliating layers into glauconite rods. The product after that was extracted by filtration using Whitman filter paper, washed several times with distilled water, and finally dried at 60 °C to be applied in further characterization steps.

4.3. Characterization Instruments

The crystal forms and crystallization properties were assessed and analyzed based on the X-ray diffraction (XRD) patterns of the prepared materials using a PANalytical-Empyrean X-ray diffractometer with a detection range spanning from 0 to 70°. The change in the structural chemical groups during the production steps was estimated using a Shimadzu FTIR-8400S spectrometer covering the detection range of 400 until 4000 cm–1. The surficial characteristics of the resulting structures, together with the initial glauconite, were analyzed using a Gemini Zeiss Ultra 55 scanning electron microscopy. The materials being studied were made ready by spraying their surfaces with gold films immediately before imaging. Moreover, their internal structures and scrolling features were subsequently observed using HRTEM photos, which were gathered employing a transmission electron microscope (JEOL-JEM2100) with an accelerating voltage of 200 kV. The degrees of porosity along with specific surface area were determined by employing a surface area analyzer (Beckman Coulter SA3100) immediately following the degassing of the specimens. The assessment has been accomplished based on the well-established N2 adsorption and desorption isotherms.

4.4. Batch MG Adsorption Experiments

The adsorption tests of MG dye by the synthetic GNRs were studied in batch form considering the impact of pH (2–9), dye concentration (100–1000 mg/L), and adsorption duration (30–900 min). These tests were performed in triplicate considering the fixed volume of the treated dye solutions (100 mL) and certain GNR dosages (0.2 g/L). The adsorption equilibrium tests were assessed at different temperature conditions (308, 318, and 323 K). By completing the equilibration interval of each test, the water samples after the tests were filtrated by Whitman filter paper (40 μm) to remove the incorporated GNR fractions and to test the remaining concentration of the dye in the solutions. The remaining MG concentrations after the treatment steps were determined using a UV–vis spectrophotometer, and the values were applied in the calculation of the MG adsorption capacity of GNRs according to eq 5. The Qe, Co, Ce, V, and m symbols in the equation identify the GNR adsorption capacity (mg/g), starting MG concentration (mg/L), rest MG concentration (mg/L), tested volume of MG aqueous solution (mL), and GNR dosage (mg).
Qe(mg/g)=(Co−Ce)Vm
(5)

4.5. Conventional and Modern Equilibrium Investigations

The adsorption of MG via GNRs were illustrated according to the commonly applied classic kinetics, classic isotherm, and advanced isotherm studies based on the theoretical statistical physics theory (Table S1). The studied kinetic and traditional isotherm models were evaluated based on the recognized nonlinear fitting degrees of the performed MG adsorption results, considering the values of both the determined coefficient (R2) (eq 6) and chi-square (χ2) (eq 7). About the nonlinear fit levels involving the simulated isotherm models’ explanatory formulas and the MG decontamination findings, they were assessed on the basis of both the determination coefficient (R2) and root-mean-square error (RMSE) (eq 8). The incorporated m′, p, Qical, and Qiexp in the equation refer to the MG uptake results, uptake parameters, calculated MG uptake capacity, and measured MG uptake capacity, respectively.
R2=1−∑(Qe,exp−Qe,cal)2∑(Qe,exp−Qe,mean)2
(6)
χ2=∑(Qe,exp−Qe,cal)2Qe,cal
(7)
RMSE=∑i=1m(Qical−Qiexp)2m′−p
(8)

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsomega.3c07870.

  • Representative equations of the kinetic and isotherm models (Table S1) (PDF)

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Author Information

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  • Corresponding Authors
    • Wail Al Zoubi - Materials Electrochemistry Laboratory, School of Materials Science and Engineering, Yeungnam University, Gyeongsan 38541, Republic of Korea;  Orcidhttps://orcid.org/0000-0003-4213-8481;  Email: [email protected]
    • Mostafa R. Abukhadra - Materials Technologies and their Applications Lab, Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt;  Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt;  Orcidhttps://orcid.org/0000-0001-5404-7996;  Email: [email protected]
  • Authors
    • Aya Fadl Allah - Materials Technologies and their Applications Lab, Geology Department, Faculty of Science, Beni-Suef University, Beni-Suef City 62511, Egypt;  Department of Chemistry, Faculty of Science, Beni-Suef University, Beni-Suef City 62514, Egypt
    • Ahmed A. Abdel-Khalek - Department of Chemistry, Faculty of Science, Beni-Suef University, Beni-Suef City 62514, Egypt
    • Ahmed M. El-Sherbeeny - Industrial Engineering Department, College of Engineering, King Saud University, P.O. Box 800, Riyadh 11421, Saudi Arabia;  Orcidhttps://orcid.org/0000-0003-3559-6249
  • Author Contributions

    This article was written through the contributions of all authors. All authors have given approval to the final version of the manuscript.

  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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This publication is funded through the United States Agency for International Development (USAID). The contents are the responsibility of the authors and do not necessarily reflect the views of USAID or the United States Government. Also, the authors extend their appreciation to King Saud University for funding this work through Researchers Supporting Project number (RSP2023R133), King Saud University, Riyadh, Saudi Arabia.

References

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This article references 75 other publications.

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  3. 3
    Abdel Salam, M.; Mokhtar, M.; Albukhari, S. M.; Baamer, D. F.; Palmisano, L.; Jaremko, M.; Abukhadra, M. R. Synthesis and Characterization of Green ZnO@polynaniline/Bentonite Tripartite Structure (G.Zn@PN/BE) as Adsorbent for As (V) Ions: Integration, Steric, and Energetic Properties. Polymers 2022, 14 (12), 2329,  DOI: 10.3390/polym14122329
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    3
    Synthesis and Characterization of Green ZnO@polynaniline/Bentonite Tripartite Structure (G.Zn@PN/BE) as Adsorbent for As (V) Ions: Integration, Steric, and Energetic Properties
    Abdel Salam, Mohamed; Mokhtar, Mohamed; Albukhari, Soha M.; Baamer, Doaa F.; Palmisano, Leonardo; Jaremko, Mariusz; Abukhadra, Mostafa R.
    Polymers (Basel, Switzerland) (2022), 14 (12), 2329CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
    A green ZnO@polynaniline/bentonite composite (G.Zn@PN/BE) was synthesized as an enhanced adsorbent for As (V) ions. Its adsorption properties were assessed in comparison with the integrated components of bentonite (BE) and polyaniline/bentonite (PN/BE) composites. The G.Zn@PN/BE composite achieved an As (V) retention capacity (213 mg/g) higher than BE (72.7 mg/g) and PN/BE (119.8 mg/g). The enhanced capacity of G.Zn@PN/BE was studied using classic (Langmuir) and advanced equil. (monolayer model of one energy) models. Considering the steric properties, the structure of G.Zn@PN/BE demonstrated a higher d. of active sites (Nm = 109.8 (20°C), 108.9 (30°C), and 67.8 mg/g (40°C)) than BE and PN/BE. This declared the effect of the integration process in inducing the retention capacity by increasing the quantities of the active sites. The no. of adsorbed As (V) ions per site (1.76 up to 2.13) signifies the retention of two or three ions per site by a multi-ionic mechanism. The adsorption energies (from -3.07 to -3.26 kJ/mol) suggested phys. retention mechanisms (hydrogen bonding and dipole bonding forces). The adsorption energy, internal energy, and free enthalpy reflected the exothermic, feasible, and spontaneous nature of the retention process. The structure is of significant As (V) uptake capacity in the existence of competitive anions or metal ions.
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  4. 4
    AlHammadi, A. A.; Nasser, R.; Shaban, M. S.; Othman, S. I.; Khim, J. S.; Ajarem, J. S.; Allam, A. A.; Abukhadra, M. R. Insight into the Effect of Sulfonation Techniques on the Adsorption Properties of – SO3H Surface-Functionalized Coal as Adsorbent for Malachite Green Dye: Steric and Energetic Investigation. ACS Omega 2022, 7 (41), 36697– 36711,  DOI: 10.1021/acsomega.2c04985
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    4
    Insight into the Effect of Sulfonation Techniques on the Adsorption Properties of -SO3H Surface-Functionalized Coal as Adsorbent for Malachite Green Dye: Steric and Energetic Investigation
    AlHammadi, Ali A.; Nasser, Rania; Shaban, Mohamed S.; Othman, Sarah I.; Khim, Jong Seong; Ajarem, Jamaan S.; Allam, Ahmed A.; Abukhadra, Mostafa R.
    ACS Omega (2022), 7 (41), 36697-36711CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    Natural coal (N.C) was sulfonated with sulfuric acid by normal stirring (MS.C) and sonication waves (SS.C) to obtain -SO3H functionalized coal as enhanced adsorbents of malachite green dye (MG). The sulfonated products exhibit enhanced surface area MS.C (27.2 m2/g) and SS.C (45.8 m2/g) as compared to N.C. SS.C achieved higher acid d. (14.2 mmol/g) and sulfur content (13.2 wt. %) as compared to MS.C. The impact of the sulfonation processes on the adsorption of MG was assessed based on the monolayer isotherm model of one energy. The MG Qsat of N.C (121.3 mg/g), MS.C (226.3 mg/g), and SS.C (296.4 mg/g) validate the significant effect of the sulfonation processes by the sonication waves. This is in agreement with the active site densities that reflect the satn. of SS.C by more active sites (180.74 mg/g) than MS.C (120.38 mg/g) and N.C (70.84 mg/g). The MS.C and SS.C can adsorb three MG mols. as compared to two mols. per site of N.C. The Gaussian energy (<8 kJ/mol) and adsorption energy (<40 kJ/mol) reflects the physisorption of MG involving van der Waals forces, hydrogen bonding, and dipole bonding forces. The thermodn. functions demonstrate the uptake of MG by exothermic, spontaneous, feasible reactions.
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  5. 5
    Benisha, R.; Amalanathan, M.; Aravind, M.; Mary, M. S. M.; Ahmad, A.; Tabassum, S.; Al-Qahtani, W. H.; Ahmad, I. Catharanthus Roseus Leaf Extract Mediated Ag-MgO Nanocatalyst for Photocatalytic Degradation of Congo Red Dye and Their Antibacterial Activity. J. Mol. Struct. 2022, 1262, 133005  DOI: 10.1016/j.molstruc.2022.133005
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    5
    Catharanthus roseus leaf extract mediated Ag-MgO nanocatalyst for photocatalytic degradation of Congo red dye and their antibacterial activity
    Benisha, R.; Amalanathan, M.; Aravind, M.; Mary, M. Sony Michel; Ahmad, Awais; Tabassum, Sobia; Al-Qahtani, Wahidah H.; Ahmad, Ikram
    Journal of Molecular Structure (2022), 1262 (), 133005CODEN: JMOSB4; ISSN:0022-2860. (Elsevier B.V.)
    A simple and cost-effective green synthesis approach was used for the manuf. of MgO and Ag-MgO nanocomposites using Catharanthus roseus leaf ext. and its photocatalytic ability against congo red (CR) dye was investigated. UV-visible spectroscopy (UV-Vis), Fourier transform IR spectroscopy (FTIR), X-ray difraction (XRD), transmission electron microscope (TEM), energy-dispersive X-ray spectroscopy (EDX), and XPS were used to examine the synthesized MgO NPs and Ag-MgO nanocomposite. The XRD pattern of MgO nanoparticles and Ag-MgO nanocomposites reveals fcc structure. Spherical shaped NPs were confirmed using SEM and TEM anal. The EDX profile confirmed the presence of Mg, Ag, and O elements. The existence of functional group responsible for stabilizing Ag-MgO nanocomposite was verified using FTIR anal. According to XPS spectra, valencies and binding energies of MgO and Ag elements were found in the as-prepd. Ag-MgO nanocomposites. Ag-MgO NCs degraded congo red (CR) dye faster than pure MgO NPS under sunlight irradn. than pure MgO NPs. The effect of dopant concn. on lowering recombination between electrons and holes was linked to increased photocatalytic activity of Ag-MgO NCs. Antibacterial results show good antibacterial activity against gram-pos. (S. aureus) and gram-neg. (E-Coli) microbial pathogens. These findings revealed the environmental remediation potential of Ag-doped MgO NPs.
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  6. 6
    Taher, T.; Putra, R.; Rahayu Palapa, N.; Lesbani, A. Preparation of Magnetite-Nanoparticle-Decorated NiFe Layered Double Hydroxide and Its Adsorption Performance for Congo Red Dye Removal. Chem. Phys. Lett. 2021, 777, 138712  DOI: 10.1016/j.cplett.2021.138712
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    6
    Preparation of magnetite-nanoparticle-decorated NiFe layered double hydroxide and its adsorption performance for congo red dye removal
    Taher, Tarmizi; Putra, Raden; Rahayu Palapa, Neza; Lesbani, Aldes
    Chemical Physics Letters (2021), 777 (), 138712CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
    Magnetite-nanoparticle-decorated NiFe LDH (MNPs@NiFe LDH) has been synthesized by the copptn. method followed by subsequent hydrothermal treatment. Material characterization was conducted using XRD, FTIR, SEM, BET surface area, and TG-DTA. MNPs@NiFe LDH exhibited high crystallinity, where the MNPs are uniformly distributed on its surface. MNPs@NiFe LDH showed higher adsorption capacity for congo red dye removal from an aq. soln. (79.6 mg/g). A further adsorption study, kinetics, isotherm, and thermodn. indicated that the adsorption mechanism is governed by ionic interaction between the pos. charged surface of the LDH and neg. charged dye mols.
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  7. 7
    Okasha, A. T.; Abdel-Khalek, A. A.; El-Sherbeeny, A. M.; Zoubi, W. A.; Abukhadra, M. R. Advanced Equilibrium Study on the Synthesis and Characterization of Mg-Doped Hydroxyapatite Nano-Fibers as a Potential Enhanced Adsorbent of Zn (II) and Malachite Green Dye. Materials Today Communications 2023, 35, 105883  DOI: 10.1016/j.mtcomm.2023.105883
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    7
    Advanced equilibrium study on the synthesis and characterization of Mg-doped hydroxyapatite nano-fibers as a potential enhanced adsorbent of Zn (II) and malachite green dye
    Okasha, Alaa T.; Abdel-Khalek, Ahmed A.; El-Sherbeeny, Ahmed M.; Zoubi, Wail Al; Abukhadra, Mostafa R.
    Materials Today Communications (2023), 35 (), 105883CODEN: MTCAC7; ISSN:2352-4928. (Elsevier Ltd.)
    Novel Mg-doped hydroxyapatite nanofibers (Mg.HAPNFs) were synthesized using inexpensive natural phosphorite and a facile method. The as-synthesized Mg.HAPNFs were characterized using several anal. methods and used as excellent adsorbent for Zn2+ ions and malachite green (MG) dye. The exptl. adsorption capacities of the as-synthesized Mg.HAPNFs for Zn2+ ions and MG dye were 441.2 and 635.1 mg/g, resp., whereas the theor. adsorption capacities at satn. were 458.7 and 673.5 mg/g, resp. The kinetics of the Mg.HAPNFs adsorption reactions for Zn2+ ions and MG dye were described using the pseudo-first-order kinetic model. A homogeneous monolayer mechanism for the adsorption of Zn2+ ions and MG dye mols. onto Mg.HAPNFs was proposed by fitting the exptl. data with the theor. Langmuir isotherm. The advanced equil. study of the Mg.HAPNF-Zn2+ and Mg.HAPNF-MG adsorption systems demonstrated that each active site of Mg.HAPNF vertically adsorbed three Zn2+ ions (n = 2.04) and two MG dye mols. (n = 1.92) via multi-ionic processes. The effective d. of adsorption sites of Mg.HAPNFs for MG dye (547.78 mg/g) was higher than that for Zn2+ ions (224.56 mg/g). The Gaussian energies (4.20 kJ/mol (Zn2+ ions) and 5.37 kJ/mol (MG dye)), adsorption energies (-5.4 kJ/mol (Zn2+ ions) and - 17.85 kJ/mol (MG dye)), and exptl. data for the Mg.HAPNF adsorbent indicated that adsorption involved several phys. and chem. mechanisms (i.e., hydrogen bonding, dissoln.-pptn., van der Waals forces, ion exchange, and dipole-dipole interactions). Thermodn. studies revealed that Mg.HAPNFs spontaneously and exothermically adsorbed Zn2+ ions and MG dye mols.
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  8. 8
    Pathania, D.; Dhar, S.; Sharma, A.; Srivastava, A. K. Decolourization of Noxious Safranin-T from Waste Water Using Mangifera Indica as Precursor. Environmental Sustainability 2021, 4 (2), 355– 364,  DOI: 10.1007/s42398-020-00130-0
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    8
    Decolourization of noxious safranin-T from waste water using Mangifera indica as precursor
    Pathania, Deepak; Dhar, Sunil; Sharma, Arush; Srivastava, A. K.
    Environmental Sustainability (2021), 4 (2), 355-364CODEN: ESNUAP; ISSN:2523-8922. (Springer)
    Abstr.: Bark prepd. from Mangifera indica has been employed for eradication of safranin-T. Structural anal. of bark was attempted using Fourier-transform IR spectroscopy (FTIR), thermogravimetric anal. (TGA), and SEM (SEM). The effect of several parameters was tested and optimized. The percentage adsorption of dye onto bark was found to increase with temp. and dictate endothermic adsorption. About 87% of dye removal was found at contact time of 80 min. The percentage of safranin-T dye removal increased with adsorbent dosage. Different isotherms like Langmuir, Freundlich, and Tempkin were studied to det. the adsorption mechanism. The adsorption capacity of bark was recorded to be 78.96 mg/g. Langmuir model rightly described the adsorption process with higher regression value (R2 = 0.99). The exptl. data was found close to using Langmuir isotherm. This confirms the monolayer adsorption of safranin-T dye onto bark. The kinetic study and intra-particle diffusion described that adsorption followed the pseudo-second-order kinetics with greater R2 value. The study confirmed the chem. adsorption of dye onto adsorbent. The different thermodn. processes confirmed the feasible, spontaneous and endothermic adsorption of dye using M. indica bark. Graphic abstr.: [graphic not available: see fulltext].
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  9. 9
    Abukhadra, M. R.; Mostafa, M.; El-Sherbeeny, A. M.; El-Meligy, M. A.; Nadeem, A. Instantaneous Adsorption of Synthetic Dyes from an Aqueous Environment Using Kaolinite Nanotubes: Equilibrium and Thermodynamic Studies. ACS Omega 2021, 6 (1), 845– 856,  DOI: 10.1021/acsomega.0c05430
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    9
    Instantaneous adsorption of synthetic dyes from an aqueous environment using kaolinite nanotubes: Equilibrium and thermodynamic studies
    Abukhadra, Mostafa R.; Mostafa, Merna; El-Sherbeeny, Ahmed M.; El-Meligy, Mohammed A.; Nadeem, Ahmed
    ACS Omega (2021), 6 (1), 845-856CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    Innovative kaolinite nanotubes (KNTs) are synthesized utilizing a simple technique involving a sonication-induced exfoliation process, followed by chem. scrolling reactions. The KNTs as a material have high reactivity and promising surface area to be used in the purifn. of water from cationic dyes (safranin (SF) and malachite green (MG)) and anionic dyes (methyl orange (MO) and Congo red (CR)). The kinetic studies of the four dyes SF, MG, CR, and MO show an equilibration time interval of 240 min. The SF, MG, CR, and MO dyes' uptake reactions are in agreement with the kinetic behavior of the pseudo-first-order model and the equil. properties of the Langmuir model. Such modeling results, in addn. to the Gaussian energies from the Dubinin-Radushkevich (D-R) model (SF (1.01 kJ/mol), MG (1.08 kJ/mol), CR (1.11 kJ/mol), and MO (1.65 kJ/mol)), hypothesize monolayer adsorption of the four dyes by phys. reactions. The KNTs show theor. qmax values of 431.6, 489.9, 626.2, and 675.5 (mg/g) for SF, MG, CR, and MO, resp. The thermodn. examn. of SF, MG, CR, and MO adsorption reactions using KNTs verifies their adsorption by exothermic and spontaneous reactions. The KNT adsorbents achieve promising adsorption results in the presence of different coexisting ions and show significant recyclability properties. Therefore, the prodn. of KNTs from kaolinite shows a strong effect on inducing the textural, physicochem., and adsorption properties of clay layers as well as their affinity for different species of synthetic dyes.
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  10. 10
    Mohamed, F.; Abukhadra, M. R.; Shaban, M. Removal of Safranin Dye from Water Using Polypyrrole Nanofiber/Zn-Fe Layered Double Hydroxide Nanocomposite (Ppy NF/Zn-Fe LDH) of Enhanced Adsorption and Photocatalytic Properties. Science of The Total Environment 2018, 640–641, 352– 363,  DOI: 10.1016/j.scitotenv.2018.05.316
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    10
    Removal of safranin dye from water using polypyrrole nanofiber/Zn-Fe layered double hydroxide nanocomposite (Ppy NF/Zn-Fe LDH) of enhanced adsorption and photocatalytic properties
    Mohamed, Fatma; Abukhadra, Mostafa R.; Shaban, Mohamed
    Science of the Total Environment (2018), 640-641 (), 352-363CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
    Polypyrrole nanofiber/Zn-Fe layered double hydroxide (Ppy NF/Zn-Fe LDH) was synthesized as nanocomposite of enhanced adsorption and photocatalytic properties. The formation of the composite was confirmed by XRD, FT-IR, HSEM, HRTEM, BET surface area and UV-vis spectrophotometer. Ppy NF/Zn-Fe LDH composite exhibits clear enhancing in the sp. surface area and obvious reducing in the band gap energy (from 2.8 eV for Zn-Fe LDH to 2.31 eV for the composite). This was reflected in a considerable improvement in the adsorption capacity and photocatalytic removal of safranin dye. The adsorption capacity was enhanced by about 22% higher than Ppy NF and by 31% higher than Zn-Fe LDH. The photocatalytic removal was improved by 41.6% higher than Ppy NF and by about 54% higher than Zn-Fe LDH. The adsorption of safranin dye by the composite is chemisorption adsorption and occurs in a multilayer form. The complete photocatalytic removal of 5 mg/L of safranin dye can be achieved after 120 min illumination time using 0.05 g of the composite as photocatalyst and the best results can be obtained at neutral to alk. conditions. Realistic application of the composite for the removal of dye from raw water samples revealed the applicability of the product for the purifn. of tap water, groundwater, and sewage water. Moreover, it can be used for six cycles of safranin dye removal from water. The photocatalytic degrdn. process appears to be controlled by the created hydroxyl radicals and formed photogenerated holes as the dominant active oxidizing radicals.
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  11. 11
    Eltaweil, A. S.; Ali Mohamed, H.; Abd El-Monaem, E. M.; El-Subruiti, G. M. Mesoporous Magnetic Biochar Composite for Enhanced Adsorption of Malachite Green Dye: Characterization, Adsorption Kinetics. Thermodynamics and Isotherms. Advanced Powder Technology 2020, 31 (3), 1253– 1263,  DOI: 10.1016/j.apt.2020.01.005
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  12. 12
    Rabie, A. M.; Abukhadra, M. R.; Rady, A. M.; Ahmed, S. A.; Labena, A.; Mohamed, H. S. H.; Betiha, M. A.; Shim, J.-J. Instantaneous Photocatalytic Degradation of Malachite Green Dye under Visible Light Using Novel Green Co–ZnO/Algae Composites. Res. Chem. Intermed. 2020, 46 (3), 1955– 1973,  DOI: 10.1007/s11164-019-04074-x
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    12
    Photocatalytic degradation of malachite green under visible light using green Co-ZnO/algae composites
    Rabie, Abdelrahman M.; Abukhadra, Mostafa R.; Rady, Ahmed M.; Ahmed, Sayed A.; Labena, Ahmed; Mohamed, Hussein S. H.; Betiha, Mohamed A.; Shim, Jae-Jin
    Research on Chemical Intermediates (2020), 46 (3), 1955-1973CODEN: RCINEE; ISSN:0922-6168. (Springer)
    Abstr.: Nano-ZnO and Co-ZnO supported algae (Sargassum species) were synthesized as a novel composite of promising photocatalytic activities in decolorization of malachite green dye under a visible light source. The composites were characterized by different anal. techniques, and the results confirmed the loading process and the formation of composites of low band gap energies for ZnO/algae composite (2.45 eV) and Co-ZnO/algae composite (2.32 eV). The composites were used as photocatalysts for the rapid degrdn. of malachite green dye (MG) within the visible light zone. The synthetic catalysts showed stunning photocatalytic activities reflected in the complete degrdn. of 5 mg/L of MG after 10 min using 0.06 g of ZnO/algae and 0.05 g of Co-ZnO/algae at pH 7. Also, the studied composites showed high efficiency in the degrdn. of higher MG concn. (10 mg/L and 15 mg/L). The photocatalytic performances were enhanced by 58% for ZnO/algae and about 75% for Co-ZnO/algae as compared to pure ZnO without support. Moreover, they have high reusability properties and are applied effectively in seven cycles of MG degrdn. reusing tests. The active species trapping tests reflected the dominance of the electron-hole pairs in the visible light degrdn. of MG by ZnO/algae. For Co-ZnO/algae composite, the degrdn. mechanism appears to be controlled by both the electron-hole pairs and hydroxyl radicals with a similar effect.
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  13. 13
    Saad, A. M.; Abukhadra, M. R.; Abdel-Kader Ahmed, S.; Elzanaty, A. M.; Mady, A. H.; Betiha, M. A.; Shim, J.-J.; Rabie, A. M. Photocatalytic Degradation of Malachite Green Dye Using Chitosan Supported ZnO and Ce–ZnO Nano-Flowers under Visible Light. Journal of Environmental Management 2020, 258, 110043  DOI: 10.1016/j.jenvman.2019.110043
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    13
    Photocatalytic degradation of malachite green dye using chitosan supported ZnO and Ce-ZnO nano-flowers under visible light
    Saad, Alaa Magdy; Abukhadra, Mostafa R.; Abdel-Kader Ahmed, Sayed; Elzanaty, Ali M.; Mady, Amr H.; Betiha, Mohamed A.; Shim, Jae-Jin; Rabie, Abdelrahman M.
    Journal of Environmental Management (2020), 258 (), 110043CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
    Two types of chitosan-based composites (chitosan/ZnO and chitosan/Ce-ZnO composites) were synthesized under microwave irradn. and characterized as advanced catalysts of enhanced photocatalytic activity under the visible light. The morphol. investigation reflected the formation of ZnO and Ce doped ZnO at stunning micro flowers of nano limps. Addnl., the optical studies reflected a redn. in the bandgap of ZnO from 3.3 eV to 2.85 eV and 2.5 eV after supporting it onto chitosan chains and after doping it with cerium, resp. The synthetic composites were applied in photocatalytic removal of malachite green dye under a visible light source. The synthetic CH/ZnO and CH/Ce-ZnO showed enhancement in the photocatalytic removal of M. G by 54% and 87%, resp., as compared to the pure ZnO. The synthetic composites are of high stability and can be reused for five photocatalytic degrdn. cycles at stunning removal percentages. The main oxidizing radicals during the removal of M. G by CH/ZnO are the generated electron-hole pairs as well as the hydroxyl radicals. The effective species in CH/Ce-ZnO photocatalytic system are the photogenerated hydroxyl radicals followed by the electron-hole pairs.
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  14. 14
    Ofudje, E. A.; Adedapo, A. E.; Oladeji, O. B.; Sodiya, E. F.; Ibadin, F. H.; Zhang, D. Nano-Rod Hydroxyapatite for the Uptake of Nickel Ions: Effect of Sintering Behaviour on Adsorption Parameters. Journal of Environmental Chemical Engineering 2021, 9 (5), 105931  DOI: 10.1016/j.jece.2021.105931
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    14
    Nano-rod hydroxyapatite for the uptake of nickel ions: Effect of sintering behaviour on adsorption parameters
    Ofudje, Edwin Andrew; Adedapo, Adebusayo Emmanuel; Oladeji, Olugbenga Bowale; Sodiya, Ezekiel Folorunso; Ibadin, Francis Hope; Zhang, Dan
    Journal of Environmental Chemical Engineering (2021), 9 (5), 105931CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
    Sorption studies in batch approach were carried out to investigate the elimination of Ni(II) ions from aq. soln. by fish scale derived nano-rod hydroxyapatite (FSDNHA) obtained via thermal decompn. at 800 and 900 oC resp. The effects of Ni2+ concn., contact time, pH, FSDNHA dose and temp. on elimination process were examd. Adsorption studies showed that max. uptake amt. of Ni2+ was attained at initial Ni2+concn. of 240 mg L-1, sorption time of 120 min, FSDNHA dose of 40 mg and soln. pH of 6.0. The highest value of R2 obtained for Langmuir, Temkin, and Freundlich isotherms models are (0.996, 0.994, and 0.990) for FSDNHA-800 and (0.998, 0.986, and 0.992) for FSDNHA-900 resp. The values of the max. monolayer adsorption capacities obtained from Langmuir isotherm for FSDNHA-800 and FSDNHA-900 are 114.151 and 183.321 mg g-1 resp. Kinetic modeling of the adsorption data clearly revealed that the sorption of Ni2+ onto the active sites of the FSDNHA surface was governed by Pseudo-first-order kinetic model. Thermodn. parameters of Gibbs free energy (ΔG°), enthalpy (ΔH°) and entropy change (ΔS°) revealed that the sorption of Ni2+on FSDNHA was spontaneous, feasible and exothermic in nature. Well resolved peaks of a characteristic pure hydroxyapatite (HA) contg. hydroxyl, phosphate and carbonate groups were obtained as the major functional groups responsible for the uptake of Ni2+, while the morphol. anal. by FE-SEM and TEM revealed a nano-rod shape. This current study showed that Ni2+ removal by FSDNHA compared favorable with other adsorbents and is feasible.
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  15. 15
    Shahid, M.; Farooqi, Z. H.; Begum, R.; Arif, M.; Irfan, A.; Azam, M. Extraction of Cobalt Ions from Aqueous Solution by Microgels for In-Situ Fabrication of Cobalt Nanoparticles to Degrade Toxic Dyes: A Two Fold-Environmental Application. Chem. Phys. Lett. 2020, 754, 137645  DOI: 10.1016/j.cplett.2020.137645
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    15
    Extraction of cobalt ions from aqueous solution by microgels for in-situ fabrication of cobalt nanoparticles to degrade toxic dyes: Two fold-environmental application
    Shahid, Muhammad; Farooqi, Zahoor H.; Begum, Robina; Arif, Muhammad; Irfan, Ahmad; Azam, Muhammad
    Chemical Physics Letters (2020), 754 (), 137645CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
    Microgels were obtained by method of free radical pptn. polymn. and characterized by TEM, DLS and FTIR. Adsorption of Co2+ ions was studied under various conditions of pH, concn. of metal ions and that of microgels. Different adsorption isotherms were applied to study mechanism of adsorption process. Kinetics and mechanism of the adsorption process was investigated by pseudo 1st order, pseudo 2nd order and intra-particle diffusion modeling. In situ redn. of Co2+ ions loaded into the polymer microgel was carried out to get hybrid system for catalytic degrdn. of 4-nitrophenol, Eosin and Methylene blue.
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  16. 16
    Sayed, I. R.; Farhan, A. M.; AlHammadi, A. A.; El-Sayed, M. I.; Abd El-Gaied, I. M.; El-Sherbeeny, A. M.; Al Zoubi, W.; Ko, Y. G.; Abukhadra, M. R. Synthesis of Novel Nanoporous Zinc Phosphate/Hydroxyapatite Nano-Rods (ZPh/HPANRs) Core/Shell for Enhanced Adsorption of Ni2+ and Co2+ Ions: Characterization and Application. J. Mol. Liq. 2022, 360, 119527  DOI: 10.1016/j.molliq.2022.119527
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    16
    Synthesis of novel nanoporous zinc phosphate/hydroxyapatite nano-rods (ZPh/HPANRs) core/shell for enhanced adsorption of Ni2+ and Co2+ ions: Characterization and application
    Sayed, Islam R.; Farhan, Amna M.; AlHammadi, Ali A.; El-Sayed, Mohamed I.; Abd El-Gaied, Ibrahim M.; El-Sherbeeny, Ahmed M.; Al Zoubi, Wail; Ko, Young Gun; Abukhadra, Mostafa R.
    Journal of Molecular Liquids (2022), 360 (), 119527CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
    Novel nanoporous zinc phosphate/hydroxyapatite nano-rods core/shell (ZPh/HPANRs) was synthesized and characterized as a modified form of hydroxyapatite with superior Ni2+ and Co2+ adsorption capacities. The ZPh/HPANRs structure exhibits satn. adsorption capacities of 515.4 mg/g (Ni2+) and 758 mg/g (Co2+). The Ni2+ and Co2+ uptake reactions by ZPh/HPANRs follow the theor. behavior of Pseudo-First order and Pseudo-Second order kinetics, resp. The assumptions of the classic Langmuir isotherm and advanced Monolayer model with one energy site were applied to illustrate the equil. properties of both Ni2+ and Co2+ uptake reactions. Considering the steric parameters, the nos. of adsorbed Ni2+ (n = 1.52-2.58) and Co2+ (n = 1.07-2.55) suggest their adsorption as two or three metal ions per each active site of ZPh/HPANRs by multi-ionic processes and in a vertical orientation. The structure show higher active site d. for the Co2+ (Nm = 702.6 mg/g) than Ni2+ ions (Nm = 339.14 mg/g). The Gaussian energies (Ni2+ (3.13-4.49 kJ/mol) and Co2+ (8.63-9.44 kJ/mol)), adsorption energies (Ni2+ (-27.3 to -28.49 kJ/mol) and Co2+ (-25.11 to -28.2 kJ/mol)), FT-IR anal. and EDX anal. demonstrate complex chem. (pptn. and chem. complexation), phys. (hydrogen bonding), and ion exchange mechanisms. The thermodn. functions display the spontaneous and exothermic properties of the Ni2+ and Co2+ uptake reactions.
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  17. 17
    Albukhari, S. M.; Salam, M. A.; Abukhadra, M. R. Effective Retention of Inorganic Selenium Ions (Se (VI) and Se (IV)) Using Novel Sodalite Structures from Muscovite; Characterization and Mechanism. Journal of the Taiwan Institute of Chemical Engineers 2021, 120, 116– 126,  DOI: 10.1016/j.jtice.2021.02.026
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    17
    Effective retention of inorganic Selenium ions (Se (VI) and Se (IV)) using novel sodalite structures from muscovite; characterization and mechanism
    Albukhari, Soha M.; Salam, Mohamed Abdel; Abukhadra, Mostafa R.
    Journal of the Taiwan Institute of Chemical Engineers (2021), 120 (), 116-126CODEN: JTICA8; ISSN:1876-1070. (Elsevier B.V.)
    Muscovite flakes were applied in the synthesis of three types of sodalite with different morphologies by hydrothermal processes for 24 h, 48 h, and 72 h. The synthetic sample after 72 h (S-72) showed the best surface area (105 m2/g), morphol. features, and ion exchange capacity (71.3 meq/100 g). The S-72 was applied for effective retention of both Se (VI) and Se (IV) ions in batch adsorption studies. The retention capacities of Se (VI) and Se (IV) ions using S-72 sodalite are 149 mg/g and 255 mg/g, resp. after an equilibration time of 300 min and 360 min. The kinetic assessment suggested Pseudo-second order behavior for the retention of both Se (VI) and Se (IV). The equil. studies of their retention reactions demonstrated Langmuir isotherm behavior and monolayer form for the homogeneously adsorbed Se (VI) and Se (IV) ions on the surface of sodalite. The Gaussian energies (> 8 KJ/mol), enthalpies (< 80 KJ/mol), and Gibbs free energies (< 40 KJ/mol) for both Se (VI) and Se (IV) suggested phys. reactions related to coulumbic attractive forces or ion exchange process. Based on the thermodn. investigations, the Se (VI) and Se (IV) retention reactions are of exothermic, favorable, and spontaneous properties. The removal percentages of Se (VI) and Se (IV) ions by sodalite in the coexisting of Pb2+, Zn2+, PO-34, and NH4+ ions are of significant values either in pH 2 or pH 7.
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  18. 18
    Raju, CH. A. I.; Anitha, J.; Mahalakshmi Kalyani, R.; Satyanandam, K.; Jagadeesh, P. Sorption of Cobalt Using Marine Macro Seaweed Graciliariacorticatared Algae Powder. Materials Today: Proceedings 2021, 44, 1816– 1827,  DOI: 10.1016/j.matpr.2020.12.009
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    18
    Sorption of cobalt using marine macro seaweed graciliariacorticatared algae powder
    Raju, CH. A. I.; Anitha, J.; Mahalakshmi Kalyani, R.; Satyanandam, K.; Jagadeesh, P.
    Materials Today: Proceedings (2021), 44 (7_Part_1), 1816-1827CODEN: MTPAC4; ISSN:2214-7853. (Elsevier Ltd.)
    Heavy metals are perilous contaminations that may exist in marine, ground, modern and even treated waste waters. Defilement of watery situations by weighty metals is an overall ecol. issue because of their poisonous impacts and their collection through the natural pecking order. Because of fast advancement of mech. exercises lately, the degrees of weighty metals in water frameworks, which have considerably expanded after some time, will prompt unnecessary arrival of the hefty metals into nature. Thus, it's important to eliminate these metals from mech. effluents before releasing watery squanders into condition. The present experimentation is aimed at removal of cobalt using gracilariacorticata red algae powder. The parameters varied are contact time, pH, sorbent size, dosage of sorbent, initial concn. and temp. The kinetics studied arelagergren first order and pseudo second order. Isotherms varied are Langmuir, Freundlich and Temkin. Optimization was carried out using Artificial neural networks and response surface methodol. The results were compared and are in good agreement.
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  19. 19
    Zhang, Y.; Hui, C.; Wei, R.; Jiang, Y.; Xu, L.; Zhao, Y.; Du, L.; Jiang, H. Study on Anionic and Cationic Dye Adsorption Behavior and Mechanism of Biofilm Produced by Bacillus Amyloliquefaciens DT. Appl. Surf. Sci. 2022, 573, 151627  DOI: 10.1016/j.apsusc.2021.151627
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    19
    Study on anionic and cationic dye adsorption behavior and mechanism of biofilm produced by Bacillus amyloliquefaciens DT
    Zhang, Yiping; Hui, Cai; Wei, Ran; Jiang, Ying; Xu, Ligen; Zhao, Yuhua; Du, Linna; Jiang, Hui
    Applied Surface Science (2022), 573 (), 151627CODEN: ASUSEE; ISSN:0169-4332. (Elsevier B.V.)
    Biofilm produced by Bacillus amyloliquefaciens DT was reported to be able to remove crystal violet from water. However, there is no report on the ability of biofilm to remove other dyes. Here, we used methyl blue (MB; anionic) and malachite green (MG; cationic) as model dyes and investigated the behaviors and mechanisms of their adsorption by bacterial biofilm. Biofilm surface morphol., functional groups, and chem. constituents were characterized. XPS and Fourier transform IR spectroscopy results demonstrated that the relevant adsorptive functional groups were C-N bond/-NH3-and C-N bond/O=P(C)-O- for MB and MG adsorption, resp. Isothermic and kinetic models revealed that biofilm adsorbs MB heterogeneously via chemisorption and intraparticle diffusion. In contrast, biofilm adsorbs MG mainly by phys. interaction. Biofilm adsorption capacities were substantially higher than those for most other adsorbents. Hence, biofilm is promising as an anionic and cationic dye adsorbent for wastewater treatment.
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  20. 20
    Çiftçi, H. Removal of Methylene Blue from Water by Ultrasound-Assisted Adsorption Using Low-Cost Bentonites. Chem. Phys. Lett. 2022, 802, 139758  DOI: 10.1016/j.cplett.2022.139758
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    20
    Removal of methylene blue from water by ultrasound-assisted adsorption using low-cost bentonites
    Ciftci, Hakan
    Chemical Physics Letters (2022), 802 (), 139758CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
    This study focused on the comparison of ultrasound-assisted (UA) and conventional (shaking or stirring) adsorption techniques, taking into account the time-dependent adsorption capacities. Six different bentonite samples were used as adsorbents, and methylene blue (MB) was used as adsorbate. Effects of pH, contact time, MB initial concn., and temp. on the UA-adsorption were also investigated. XRD analyzes showed that all the bentonite samples were mostly composed of montmorillonite clay minerals, while XRF analyzes showed that the samples contained high percentage of silicon and aluminum oxides (≥70 wt%). Maximum zeta potential values (37.1-42.1 mV) were measured at pH 12 and, to confirm this, max. adsorption capacities were also detd. at this point. Ultrasound irradn. significantly increased the adsorption capacities of all bentonite samples in the early stages. For example, the adsorption capacity of the B-1 bentonite sample was measured as 388 mg/g by UA-adsorption at the first 5th minute, while it was 286 mg/g by conventional (C) adsorption technique at the same time. All bentonite samples showed increasing adsorption capacity with increased temp. confirming endothermic reaction. Maximum adsorption capacities of B-1, B-2, B-3, B-4, B-5, and B-6 bentonite samples with the 96-100% MB removal percentages at selected conditions (pH: 11-12, temp.: 25°C, contact time: 60 min, and MB initial concns. for B-1: 800, B-2: 700, B-3,4: 650, B-5: 600, and B-6: 500 mg/L) were measured as 398, 342, 320, 296, 288, and 243 mg/g, resp. Pseudo-second-order kinetic model and Langmuir isotherm model with higher correlation coeffs. were found to be more suitable to explain the adsorption of MB cations onto bentonites. In addn., max. adsorption capacities of B-1, B-2, B-3, B-4, B-5, and B-6 samples at 25°C calcd. from Langmuir isotherm data detd. as 500, 454.5, 400, 384.6, 370, and 357.1 mg/g, resp.
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  21. 21
    Alqahtani, M. D.; Nasser, N.; AlZahrani, S. A.; Allam, A. A.; Abukhadra, M. R. Characterization of Kaolinite Single Methoxy Nano-Sheets as Potential Carriers of Oxaliplatin Drug of Enhanced Loading, Release, and Cytotoxicity Properties During the Treatment of Colorectal Cancer. Journal of Inorganic and Organometallic Polymers and Materials 2023, 33 (7), 2111– 2126,  DOI: 10.1007/s10904-023-02634-8
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    21
    Characterization of Kaolinite Single Methoxy Nano-Sheets as Potential Carriers of Oxaliplatin Drug of Enhanced Loading, Release, and Cytotoxicity Properties During the Treatment of Colorectal Cancer
    Alqahtani, Mashael D.; Nasser, Nourhan; AlZahrani, Saleha A.; Allam, Ahmed A.; Abukhadra, Mostafa R.
    Journal of Inorganic and Organometallic Polymers and Materials (2023), 33 (7), 2111-2126CODEN: JIOPAY; ISSN:1574-1443. (Springer International Publishing AG)
    Kaolinite mineral was exfoliated into single nano-sheets (EXFK) and functionalized by methanol forming novel methoxy kaolinite nanosheet (MX/EXFK) as effective carrier of oxaliplatin drug (OXP). The functionalization of EXFK notably enhanced the loading properties to 433 mg/g (MX/EXFK) instead of 304.9 mg/g (EXFK). The loading reactions by EXFK and MX/EXFK follow the Pseudo-first order kinetics (R2 > 0.94) and classic Langmuir isotherm (R2 = 0.99). MX/EXFK shows enhanced active sites d. (109.9 mg/g) as compared to 66.3 mg/g (EXFK) and each site can be loaded with 4 mols. by multi-mol. mechanism. The encapsulation energy (< 40 kJ/mol) and Gaussian energy (< 8 kJ/mol) validates the dominant phys. encapsulation mechanism of OXP. The release behavior of OXP from MX/EXFK demonstrates continuous and controlled profiles up to 100 h (pH) and 180 h (phosphate buffer). The release processes exhibit non-Fickian transport properties according to the kinetic studies and diffusion exponent values (0.52-0.61). The synthetic structures exhibit considerable cytotoxicity effect on HCT-116 cancer cell lines EXFK (71.4% cell viability); MX/EXFK (12.08% cell viability). Moreover, these carriers induce the cytotoxic effects of OXP significantly OXP/EXFK (2.04% cell viability); OXP/MX/EXFK (0.95% cell viability).
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  22. 22
    Almahri, A. The Solid-State Synthetic Performance of Bentonite Stacked Manganese Ferrite Nanoparticles: Adsorption and Photo-Fenton Degradation of MB Dye and Antibacterial Applications. Journal of Materials Research and Technology 2022, 17, 2935– 2949,  DOI: 10.1016/j.jmrt.2022.02.052
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    22
    The solid-state synthetic performance of bentonite stacked manganese ferrite nanoparticles: adsorption and photo-fenton degradation of MB dye and antibacterial applications
    Almahri, Albandary
    Journal of Materials Research and Technology (2022), 17 (), 2935-2949CODEN: JMRTAL; ISSN:2238-7854. (Elsevier B.V.)
    The development of nanocomposites for environmental demands is a challenge due to numerous precautions, including tailoring recyclable agents. In this work, bentonite clay (B. Clay)/manganese ferrite (MnFe2O4) nanocomposites have been fabricated via a solid-state technique that is green, efficient, and scalable. The obtained composites have been characterized using FTIR, SEM, and TEM. From the results, MnFe2O4 was configured in spherical shape during the interaction with B. Clay, reflecting the quality of applications. The studied av. max. height of the roughness (Rtm) changes from 151.7 to 107.3 and increases to 141.5 for pure B. Clay, MnFe2O4, and the nanocomposite, resp. The surface area for the nanocomposite was around 85.45 m2/g compared with 57. 46 m2/g for MnFe2O4. The magnetic domain has been enhanced exponentially to be 19.93 emu/g after solid synthesis of MnFe2O4 with B. Clay. The adsorption property was more significant in the case of MnFe2O4/B. clay to reach 71.6% decolorization of methylene blue (MB). Otherwise, under light illumination, the phytoremediation Fe3+ is reduced to Fe2+, accelerating switching on/off Fe3+/Fe2+ cycle stability to exhibit strong hydroxyl radicals able to destroy MB within 8 min. Also, at 100μg/mL concn., the prepd. MnFe2O4/B. Clay was aggressive against Staphylococcus aureus, Bacillus subtilis, Pseudomonas aeruginosa, and Escherichia coli.
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  23. 23
    Dardir, F. M.; Mohamed, A. S.; Abukhadra, M. R.; Ahmed, E. A.; Soliman, M. F. Cosmetic and Pharmaceutical Qualifications of Egyptian Bentonite and Its Suitability as Drug Carrier for Praziquantel Drug. European Journal of Pharmaceutical Sciences 2018, 115, 320– 329,  DOI: 10.1016/j.ejps.2018.01.041
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    23
    Cosmetic and pharmaceutical qualifications of Egyptian bentonite and its suitability as drug carrier for Praziquantel drug
    Dardir, Fatma M.; Mohamed, Aya S.; Abukhadra, Mostafa R.; Ahmed, Ezzat A.; Soliman, Mamdouh F.
    European Journal of Pharmaceutical Sciences (2018), 115 (), 320-329CODEN: EPSCED; ISSN:0928-0987. (Elsevier B.V.)
    The aim of this paper is to characterize and evaluate newly discovered bentonite deposits in Egypt for pharmaceutical and cosmetic applications as well as its suitability as carrier for Praziquantel drug. The study was performed for the raw bentonite sample, purified bentonite sample and alkali activated purified bentonite sample. The raw bentonite sample composed mainly of montmorillonite contaminated by little amts. of quartz and calcite, while the purified sample composed of montmorillonite without detected mineral impurities and matches the mineralogical properties of Wyoming bentonite as an international std. Geochem., the studied raw and purified samples appear to high purity with a chem. compn. close to those of Wyoming bentonite and match the pharmacopeia specifications. The chem. properties in addn. to the textural properties of the surface area, porosity, particle size distribution qualify the bentonite products to use as a function in powder, emulsion and creams. Investigation of pharmacopeia properties of pH, sedimentation vol. and swelling capacity revealed the suitability of the raw and purified samples for pharmaceutical and cosmetic applications. Moreover, the microbiol. tests indicated that the samples free from harmful microbial pathogens. At the optimum conditions of time (240 min), bentonite dose (250 mg) and reaction temp. (60°C), the obtained encapsulation percentages of Praziquantel drug are 62%, 78.4% and 93.2% for raw bentonite, purified and alkali activated bentonite, resp. The releasing percentage of the drug using an intestinal buffer at pH 7.4 is more efficient and the max. obtained values were obtained after 420 min. The obtained releasing values are 71%, 79.2% and 87.4% for raw bentonite, purified bentonite and alkali activated bentonite, resp.
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  24. 24
    Alqahtani, M. D.; Nasser, N.; Bin Jumah, M. N.; AlZahrani, S. A.; Allam, A. A.; Abukhadra, M. R.; Bellucci, S. Insight into the Morphological Properties of Nano-Kaolinite (Nanoscrolls and Nanosheets) on Its Qualification as Delivery Structure of Oxaliplatin: Loading, Release, and Kinetic Studies. Molecules 2023, 28 (13), 5158,  DOI: 10.3390/molecules28135158
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    24
    Insight into the Morphological Properties of Nano-Kaolinite (Nanoscrolls and Nanosheets) on Its Qualification as Delivery Structure of Oxaliplatin: Loading, Release, and Kinetic Studies
    Alqahtani, Mashael Daghash; Nasser, Nourhan; Bin Jumah, May N.; AlZahrani, Saleha A.; Allam, Ahmed A.; Abukhadra, Mostafa R.; Bellucci, Stefano
    Molecules (2023), 28 (13), 5158CODEN: MOLEFW; ISSN:1420-3049. (MDPI AG)
    Natural kaolinite underwent advanced morphol.-modification processes that involved exfoliation of its layers into sepd. single nanosheets (KNs) and scrolled nanoparticles as nanotubes (KNTs). Synthetic nanostructures have been characterized as advanced and effective oxaliplatin-medication (OXAP) delivery systems. The morphol.-transformation processes resulted in a remarkable enhancement in the loading capacity to 304.9 mg/g (KNs) and 473 mg/g (KNTs) instead of 29.6 mg/g for raw kaolinite. The loading reactions that occurred by KNs and KNTs displayed classic pseudo-first-order kinetics (R2 > 0.90) and conventional Langmuir isotherms (R2 = 0.99). KNTs exhibit a higher active site d. (80.8 mg/g) in comparison to KNs (66.3 mg/g) and raw kaolinite (6.5 mg/g). Furthermore, compared to KNs and raw kaolinite, each site on the surface of KNTs may hold up to six mols. of OXAP (n = 5.8), in comparison with five mols. for KNs. This was accomplished by multi-mol. processes, including phys. mechanisms considering both the Gaussian energy (<8 KJ/mol) and the loading energy (<40 KJ/mol). The release activity of OXAP from KNs and KNTs exhibits continuous and regulated profiles up to 100 h, either by KNs or KNTs, with substantially faster characteristics for KNTs. Based on the release kinetic investigations, the release processes have non-Fickian transport-release features, indicating cooperative-diffusion and erosion-release mechanisms. The synthesized structures have a significant cytotoxicity impact on HCT-116 cancer cell lines (KNs (71.4% cell viability and 143.6 g/mL IC-50)); KNTs (11.3% cell viability and 114.3 g/mL IC-50). Addnl., these carriers dramatically increase OXAPs cytotoxicity (2.04% cell viability, 15.4 g/mL IC-50 (OXAP/KNs); 0.6% cell viability, 4.5 g/mL IC-50 (OXAP/KNTs)).
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  25. 25
    Singh, R.; Dutta, S. The Role of pH and Nitrate Concentration in the Wet Chemical Growth of Nano-Rods Shaped ZnO Photocatalyst. Nano-Structures & Nano-Objects 2019, 18, 100250,  DOI: 10.1016/j.nanoso.2019.01.009
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    25
    The role of pH and nitrate concentration in the wet chemical growth of nano-rods shaped ZnO photocatalyst
    Singh, Rohini; Dutta, Suman
    Nano-Structures & Nano-Objects (2019), 18 (), 100250CODEN: NNAAH5; ISSN:2352-507X. (Elsevier B.V.)
    ZnO nano-rods were synthesized via wet chem. method at different nitrate concn. and pH value. The effect of pH and nitrate concn. on the size and morphol. of the prepd. ZnO photocatalysts have been investigated by particle size distribution anal. and Field emission SEM resp. Addnl., UV-Visible spectroscopy and energy dispersive studies and were carried out to confirm the optical and compositional properties of the prepd. ZnO powder. The estd. band gap of the as prepd. ZnO photocatalysts at different pH and nitrate concn. calcd. on the basis of Kubelka-Munk function was found to be in the range of ∼ 2.7-3.6 eV. Field emission scanning (FE-SEM) and transmission electron microscopic (TEM) observations reveal rod-like morphol. The photocatalytic activity of prepd. ZnO photocatalysts was evaluated by photo degrdn. of the mixt. of Methylene Blue (MB) and Rhodamine 6G (Rh 6G) soln. under simulated solar radiation. Vol. of hydrogen evolution was recorded in the presence of prepd. ZnO photocatalysts in 2 h. Nitrate concn., and pH value showed a significant effect on the optical and morphol. behavior of the prepd. ZnO powd. photocatalysts.
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  26. 26
    Tan, D.; Yuan, P.; Dong, F.; He, H.; Sun, S.; Liu, Z. Selective Loading of 5-Fluorouracil in the Interlayer Space of Methoxy-Modified Kaolinite for Controlled Release. Appl. Clay Sci. 2018, 159, 102– 106,  DOI: 10.1016/j.clay.2017.04.008
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    26
    Selective loading of 5-fluorouracil in the interlayer space of methoxy-modified kaolinite for controlled release
    Tan, Daoyong; Yuan, Peng; Dong, Faqin; He, Hongping; Sun, Shiyong; Liu, Zongwen
    Applied Clay Science (2018), 159 (), 102-106CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
    Methoxy-modified kaolinite was used as a novel carrier for anticancer drug 5-fluorouracil (5FU). The selective loading of 5FU into the interlayer space of methoxy-modified kaolinite was achieved because the weakly bonded 5FU on the external surface was removed off by facile water rinse. The intercalated 5FU has strong affinity (electrostatic force and hydrogen bonding) with the interlayer surface of kaolinite, and its release was controlled because of the diffusion restriction of the kaolinite lamellar layers and the strong affinity between 5FU and kaolinite. The controlled release of 5FU from methoxy-modified kaolinite in simulated colonic fluid (pH 5.5) makes it be of potential use to administer an oral formulation of 5FU for colon specific delivery.
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  27. 27
    Abukhadra, M. R.; Mohamed, A. S.; El-Sherbeeny, A. M.; Soliman, A. T. A. Enhanced Adsorption of Toxic and Biologically Active Levofloxacin Residuals from Wastewater Using Clay Nanotubes as a Novel Fixed Bed: Column Performance and Optimization. ACS Omega 2020, 5 (40), 26195– 26205,  DOI: 10.1021/acsomega.0c03785
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    27
    Enhanced adsorption of toxic and biologically active levofloxacin residuals from wastewater using clay nanotubes as a novel fixed bed: Column performance and optimization
    Abukhadra, Mostafa R.; Mohamed, Aya S.; El-Sherbeeny, Ahmed M.; Soliman, Ahmed Tawhid Ahmed
    ACS Omega (2020), 5 (40), 26195-26205CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    Kaolinite nanotube particles (KNTs) were synthesized by a chem. exfoliation and scrolling process in the existence of sonication waves. The KNT product was identified as a mesoporous material (12 nm in pore diam.) with high surface area (105 m2/g) and promising adsorption affinity for the levofloxacin antibiotic (LVOX) residuals in wastewater. The KNT particles were used as a fixed bed in the continuous adsorption column system for LVOX considering the essential variables. The investigation of the KNT fixed bed in a continuous column for 1800 min verified its suitability to reduce the LVOX content in 9 L of polluted solns. by 80.4%. This was recognized after using the KNT bed of 4 cm in height, a flow rate of 5 mL/min, a pH value of 8, a total flow interval of 1800 min, and an LVOX concn. of 10 mg/L. The regeneration study of the bed declared effective recyclability properties for the KNT particles in the LVOX adsorption column system. The dynamic properties of the KNT bed-based column system were explained based on Thomas, Adams-Bohart, and the Yoon-Nelson kinetic models. The LVOX adsorption reaction by KNTs follows Langmuir behavior with homogeneous and monolayer uptake form. The Gaussian energy (2.05 kJ/mol) and the thermodn. parameters emphasized phys., spontaneous, and exothermic adsorption reactions for LVOX by KNTs.
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  28. 28
    Guha, A.; Chattoraj, S. L.; Chatterjee, S.; Kumar, K. V.; Rao, P. V. N.; Bhaumik, A. K. Reflectance Spectroscopy-Guided Broadband Spectral Derivative Approach to Detect Glauconite-Rich Zones in Fossiliferous Limestone, Kachchh Region, Gujarat, India. Ore Geol. Rev. 2020, 127, 103825  DOI: 10.1016/j.oregeorev.2020.103825
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  29. 29
    Bruneel, Y.; Van Laer, L.; Brassinnes, S.; Smolders, E. Characterisation of the Highly Selective Caesium Sorption on Glauconite Rich Sands of Contrasting Geological Formations. Appl. Geochem. 2021, 128, 104926  DOI: 10.1016/j.apgeochem.2021.104926
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    29
    Characterisation of the highly selective caesium sorption on glauconite rich sands of contrasting geological formations
    Bruneel, Y.; Van Laer, L.; Brassinnes, S.; Smolders, E.
    Applied Geochemistry (2021), 128 (), 104926CODEN: APPGEY; ISSN:0883-2927. (Elsevier Ltd.)
    The Neogene-Paleogene glauconite sands are investigated in the framework of the Belgian radioactive waste disposal as material for an addnl. sorption sink. Glauconite is an Fe-rich phyllosilicate that is mainly present as 125-250 μm sized pellets in the sand. Recent studies have shown a surprisingly strong sorption of radiocaesium (137Cs) on these sands, despite the coarse sized pellet structure. This study was set up to characterize the selective 137Cs+ sorption sites on glauconite that are likely Frayed Edge Sites (FES) as in illite. First, the NH4/K selectivity on the FES was detd. as a fingerprint for the highly selective FES. The NH4/K selectivity coeff. on the FES for three different sand formation ranged between 3.8 and 5.0, well in line with the range (4-7) that has been reported for illite clay and clay formations. Second, the Cs+ sorption isotherms were detd. on three sand formations in a background soln. of 0.5 mM K+, 100 mM Ca+ and 10-8-10-4 M Cs+; isotherms were fitted with an optimized three-site model adapted after the illite model of Bradbury and Baeyens (2000). The optimized model fitted the data adequately. Taken together, this study suggests that the glauconite sands have highly selective sites that bind 137Cs+ with similar properties as in illite, however the fractions of these sites in the total CEC pool are about a factor five lower than in pure illite.
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  30. 30
    Singla, R.; Alex, T. C.; Kumar, R. On Mechanical Activation of Glauconite: Physicochemical Changes, Alterations in Cation Exchange Capacity and Mechanisms. Powder Technol. 2020, 360, 337– 351,  DOI: 10.1016/j.powtec.2019.10.035
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    30
    On mechanical activation of glauconite: Physicochemical changes, alterations in cation exchange capacity and mechanisms
    Singla, Rashmi; Alex, Thomas C.; Kumar, Rakesh
    Powder Technology (2020), 360 (), 337-351CODEN: POTEBX; ISSN:0032-5910. (Elsevier B.V.)
    Mech. activation (MA) of glauconite [(K,Na,Ca)(Fe3+,Al,Mg,Fe2+)2(Si,Al)4O10(OH)2] has been investigated to improve its cation exchange capacity (CEC), an impediment for its direct use as nutrients (agro-mineral), notably potassium. Glauconite is mech. activated using planetary ball milling for varying lengths of time up to 240 min. Milling induces time dependent physicochem. changes in terms of particulate characteristics (morphol., particles size distribution, geometrical and BET sp. surface area), structure (crystallite size and strain; -OH/H2O bonding) and surface charge (zeta potential). It is possible to tailor the CEC of glauconite with MA. A remarkable improvement (30-fold!) in the CEC of K+ ions is possible. The effect of milling time on the exchange behavior is ion-specific. Plausible mechanisms of cation exchange are presented in terms of the chem. nature of the ions involved and the physicochem. changes. Lastly, MA approach is compared with reported methods of potassium recovery; its superiority as a green option is underlined.
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  31. 31
    Shmandiy, V.; Rigas, T.; Kharlamova, O.; Bezdeneznych, L. Research of Adsorption Properties of Glauconite-Based Composite Adsorbents. Journal of Ecological Engineering 2020, 21 (6), 147– 154,  DOI: 10.12911/22998993/123245
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  32. 32
    Abukhadra, M. R.; Bakry, B. M.; Adlii, A.; Yakout, S. M.; El-Zaidy, M. E. Facile Conversion of Kaolinite into Clay Nanotubes (KNTs) of Enhanced Adsorption Properties for Toxic Heavy Metals (Zn2+, Cd2+, Pb2+, and Cr6+) from Water. Journal of Hazardous Materials 2019, 374, 296– 308,  DOI: 10.1016/j.jhazmat.2019.04.047
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    32
    Facile conversion of kaolinite into clay nanotubes (KNTs) of enhanced adsorption properties for toxic heavy metals (Zn2+, Cd2+, Pb2+, and Cr6+) from water
    Abukhadra, Mostafa R.; Bakry, Belal Mohamed; Adlii, Alyaa; Yakout, Sobhy M.; El-Zaidy, Mohamed A.
    Journal of Hazardous Materials (2019), 374 (), 296-308CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
    Kaolinite nanotubes (KNTs) were synthesized from kaolinite by ultrasonic scrolling and characterized using X-ray diffractometer, scanning and transmission electron microscopes; and FTIR-FT Raman spectrometer. The synthetic KNTs appear as multi-walled scrolls of 12 nm av. pore diam. and 50-600 nm particle length; and exhibit surface area of 105 m2/g. KNTs were used as adsorbents for Zn2+, Cd2+, Pb2+, and Cr6+ with uptake capacities of 103 mg/g, 116 mg/g, 89 mg/g, and 91 mg/g, resp. The equilibration time of Cd2+ and Pb2+ adsorption is 360 min and for Cr6+ and Zn2+ area 120 min and 240 min, resp. KNTs adsorption systems can be described mainly by Lagergren-second order and Freundlich models (R2> 0.95) as kinetic and isotherm models. This reflected multilayer adsorption forms with chem. sharing or ion exchange processes. KNTs exhibits high reusability and used for five cycles in the removal of the studied metals (100 mg/L). The removal percentages declined by 20.5%, 15.12%, 22.8% and 23.16% with repeating the reused cycles from cycle 1 to cycle 5 for Zn2+, Cd2+, Pb2+, and Cr6+, resp. KNTs were applied successfully in realistic purifn. of tap water, groundwater, and sewage water from the inspected metals.
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  33. 33
    Franus; Bandura; Madej Mono and Poly-Cationic Adsorption of Heavy Metals Using Natural Glauconite. Minerals 2019, 9 (8), 470,  DOI: 10.3390/min9080470
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    33
    Mono and poly-cationic adsorption of heavy metals using natural glauconite
    Franus, Malgorzata; Bandura, Lidia; Madej, Jaroslaw
    Minerals (Basel, Switzerland) (2019), 9 (8), 470CODEN: MBSIBI; ISSN:2075-163X. (MDPI AG)
    The issue of heavy metal pollution of industrial wastewaters is a major environmental concern nowadays. The aim of this study was to investigate the effectiveness of heavy metals removal from aq. solns. by natural glauconite, in batch and dynamic systems. Glauconite was characterized by X-ray diffraction, nitrogen adsorption-desorption isotherm, scanning electron microscope, DTA, and inductively coupled plasma spectroscopy. Cation exchange capacity, bulk d. and point of zero charge were also detd. In the batch system, the impact of initial concn., contact time, and pH of metal solns. on sorption efficiency was analyzed, whereas for the dynamic system, the influence of flow rate was studied. The adsorption capacity in the batch system followed the order: Pb > Cd > Zn > Cu. The highest adsorption rate was achieved in the pH range 7-9. In the column expts., the selectivity order in the case of mono-cationic system was the same as that of batch system, whereas in the case of poly-cationic system it was: Pb > Zn > Cd > Cu. With the increase of the flow rate, the total capacity at the exhaustion point increased.
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  34. 34
    Baldermann, A.; Banerjee, S.; Czuppon, G.; Dietzel, M.; Farkaš, J.; Löhr, S.; Moser, U.; Scheiblhofer, E.; Wright, N. M.; Zack, T. Impact of Green Clay Authigenesis on Element Sequestration in Marine Settings. Nat. Commun. 2022, 13 (1), 1527,  DOI: 10.1038/s41467-022-29223-6
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    34
    Impact of green clay authigenesis on element sequestration in marine settings
    Baldermann, Andre; Banerjee, Santanu; Czuppon, Gyoergy; Dietzel, Martin; Farkas, Juraj; Lohr, Stefan; Moser, Ulrike; Scheiblhofer, Esther; Wright, Nicky M.; Zack, Thomas
    Nature Communications (2022), 13 (1), 1527CODEN: NCAOBW; ISSN:2041-1723. (Nature Portfolio)
    Retrograde clay mineral reactions (reverse weathering), including glauconite formation, are first-order controls on element sequestration in marine sediments. Here, we report substantial element sequestration by glauconite formation in shallow marine settings from the Triassic to the Holocene, averaging 3 ± 2 mmol·cm-2·kyr-1 for K, Mg and Al, 16 ± 9 mmol·cm-2·kyr-1 for Si and 6 ± 3 mmol·cm-2·kyr-1 for Fe, which is ≈2 orders of magnitude higher than ests. for deep-sea settings. Upscaling of glauconite abundances in shallow-water (0-200 m) environments predicts a present-day global uptake of ≈≤ 0.1 Tmol·yr-1 of K, Mg and Al, and ≈0.1-0.4 Tmol·yr-1 of Fe and Si, which is ≈half of the estd. Mesozoic elemental flux. Clay mineral authigenesis had a large impact on the global marine element cycles throughout Earth's history, in particular during 'greenhouse' periods with sea level highstand, and is key for better understanding past and present geochem. cycling in marine sediments.
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  35. 35
    Pietsch, C.; Harrison, H. C.; Allmon, W. D. Whence the Gosport Sand (Upper Middle Eocene, Alabama)? The Origin of Glauconitic Shell Beds In the Paleogene of the U.S. Gulf Coastal Plain. Journal of Sedimentary Research 2016, 86 (11), 1249– 1268,  DOI: 10.2110/jsr.2016.72
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    35
    Whence the gosport sand (Upper Middle Eocene, Alabama)? The oriign of glauconitic shell beds in the paleogene of the U.S. Gulf Coastal Plain
    Pietsch, Carlie; Harrison, H. Cliff; Allmon, Warren D.
    Journal of Sedimentary Research (2016), 86 (11), 1249-1268CODEN: JSERFV; ISSN:1938-3681. (SEPM Society for Sedimentary Geology)
    An explanation for the depositional history of the Gosport Sand has proven to be as puzzling as its diverse mollusk fossils is beguiling. We propose that shifting delta lobes produced patchy environments which accumulated to form the Gosport Sand and likely other glauconite- and fossil-rich shell beds of the Gulf Coastal Plain of the Paleogene. We present facies and mineralogical data to suggest glauconite in the Gosport Sand was deposited during relatively stable environmental conditions. Increased glauconite maturity and taphonomic alteration in the Gosport Sand are attributed to eustatic transgression, resulting in decreased deposition, enhanced winnowing, and increased exposure at the sediment-water interface. Increased fossil diversity and abundance likely result from time averaging and accumulation of shells from ancient patchy habitats analogous to modern "inner shallow shelf" and "open sound" environments. Delta progradation and subsidence would have detd. the migration of these environments. We evoke a similar depositional model for glauconite-rich shell beds distributed throughout the Paleocene and Eocene of the Gulf Coastal Plain based on their transgressive nature and roughly equiv. facies. These shifting environmental conditions may have played a partial role in generating the high molluscan diversity of the Gulf Coastal Plain of the Paleogene.
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  36. 36
    El-Habaak, G.; Askalany, M.; Faraghaly, M.; Abdel-Hakeem, M. The Economic Potential of El-Gedida Glauconite Deposits, El-Bahariya Oasis, Western Desert. Egypt. Journal of African Earth Sciences 2016, 120, 186– 197,  DOI: 10.1016/j.jafrearsci.2016.05.007
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    Sobeih, M. M.; El-Shahat, M. F.; Osman, A.; Zaid, M. A.; Nassar, M. Y. Glauconite Clay-Functionalized Chitosan Nanocomposites for Efficient Adsorptive Removal of Fluoride Ions from Polluted Aqueous Solutions. RSC Adv. 2020, 10 (43), 25567– 25585,  DOI: 10.1039/D0RA02340J
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    37
    Glauconite clay-functionalized chitosan nanocomposites for efficient adsorptive removal of fluoride ions from polluted aqueous solutions
    Sobeih, Marwa M.; El-Shahat, M. F.; Osman, A.; Zaid, M. A.; Nassar, Mostafa Y.
    RSC Advances (2020), 10 (43), 25567-25585CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
    We herein have developed a mild approach for the fabrication of glauconite clay (G)-modified chitosan (CS) nanocomposites by the combination of a simple blending and crosslinking method. The chitosan was modified with EDTA (EDTA), glutaraldehyde (GL), sodium dodecyl sulfate (SDS), and cetyltrimethyl ammonium bromide (CTAB). The as-prepd. composites were identified using Fourier-transform IR spectroscopy (FTIR), X-ray diffraction (XRD), field emission SEM (FE-SEM), nitrogen phys. adsorption (BET), at. absorption spectrophotometry (AA), and thermal gravimetric anal. (TGA). The adsorption activities of the as-prepd. materials were assessed for the removal of fluoride ions from aq. media using a batch technique. Raw glauconite (G), GL-CS/G, SDS-CS/G, EDTA-GL-CS/G, and CTAB-CS/G adsorbents displayed max. adsorption capacity values of 1.15, 4.31, 4.55, 6.90, and 9.03 mg g-1, resp. The adsorption results were well described by employing the pseudo-second-order kinetic and Langmuir isotherm models. The estd. thermodn. consts. indicated that the F- ion adsorption was a spontaneous, physisorption process. Furthermore, the modified chitosan adsorbents are good candidates for the adsorptive elimination of F- ions from aq. solns., according to their reusability, high stability, good adsorption capacity, and applicability for actual field water samples.
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  38. 38
    Moretto, L. M.; Orsega, E. F.; Mazzocchin, G. A. Spectroscopic Methods for the Analysis of Celadonite and Glauconite in Roman Green Wall Paintings. Journal of Cultural Heritage 2011, 12 (4), 384– 391,  DOI: 10.1016/j.culher.2011.04.003
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    Shawky, A.; El-Sheikh, S. M.; Rashed, M. N.; Abdo, S. M.; El-Dosoqy, T. I. Exfoliated Kaolinite Nanolayers as an Alternative Photocatalyst with Superb Activity. Journal of Environmental Chemical Engineering 2019, 7 (3), 103174  DOI: 10.1016/j.jece.2019.103174
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    Exfoliated kaolinite nanolayers as an alternative photocatalyst with superb activity
    Shawky, Ahmed; El-Sheikh, Said M.; Rashed, Mohamed Nageeb; Abdo, Sabrin M.; El-Dosoqy, Thanaa I.
    Journal of Environmental Chemical Engineering (2019), 7 (3), 103174CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
    In searching for alternative and abundant photocatalyst, exfoliated kaolinite nanolayers (nK) were prepd. by a simple intercalation process. The effect of intercalating agents on the produced nK was studied by different instrumentations. XRD, FT-IR, and TEM confirm the exfoliation of kaolinite into nanolayers. Bandgap values were altered depending on intercalating agents as revealed by light absorption spectra. Photogenerated charge carriers obsd. through photoluminescence spectra. The produced nK applied for photodegrdn. of Rhodamine B dye (RhB) as an industrial model for wastewater treatment purposes. The results showed a complete photodegrdn. of RhB within a few minutes under UV with superb reaction kinetics. We refer the enhanced photocatalytic properties to the exposed metal oxide impurities on the surface of nK due to exfoliation. Performance tests revealed the reusability and stability of the prepd. nK. This plentiful material is supposed to be a versatile alternative for the well-known photocatalysts with the possibility of large-scale prodn. Photodegrdn. mechanism of RhB is proposed.
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  40. 40
    Younes, H.; El-Etriby, H. Kh.; Mahanna, H. High Removal Efficiency of Reactive Yellow 160 Dye from Textile Wastewater Using Natural and Modified Glauconite. International Journal of Environmental Science and Technology 2022, 19 (6), 5659– 5674,  DOI: 10.1007/s13762-021-03528-3
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    40
    High removal efficiency of reactive yellow 160 dye from textile wastewater using natural and modified glauconite
    Younes, H.; El-Etriby, H. Kh.; Mahanna, H.
    International Journal of Environmental Science and Technology (2022), 19 (6), 5659-5674CODEN: IJESHU; ISSN:1735-1472. (Springer)
    The adsorption of reactive yellow 160 (RY160) dye from textile wastewater was investigated using natural clay glauconite as an eco-friendly and low-cost adsorbent. Besides, modifications methods by thermal activation (TAG) and acid activation (AAG) of glauconite were studied to enhance the removal efficiency and adsorption capacity. Glauconite samples were characterized by FTIR spectroscopy, XRD, SEM, EDX, nitrogen adsorption/desorption isotherm, and zeta potential. Moreover, the effect of initial concn., contact time, adsorbent dose, pH, and temp. on the removal efficiency was studied. The results show that RY160 removal efficiency increases by increasing adsorbent dose. The removal efficiency reached 92.32% by raw glauconite and 100% by modified glauconite at a dose of 4 g/L. The max. adsorption of the RY160 dye is detected at pH 1.0 for raw and modified glauconite. The adsorption of RY160 on glauconite is exothermic and spontaneous. The isotherm study revealed that Freundlich isotherm fits well the exptl. data. The max. adsorption capacity improved from 29.85 mg/g for raw glauconite to 51.55 and 55.87 mg/g for TAG, and AAG, resp. The pseudo-second-order model well expresses the exptl. data (R2 = 0.997). The reusability study showed that the adsorbents could effectively regenerated and reused. The results imply that the modified glauconite could be used as a natural and low-cost adsorbent for RY160 dye removal from textile wastewater.
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  41. 41
    Salam, M. A.; Abukhadra, M. R.; Mostafa, M. Effective Decontamination of As(V), Hg(II), and U(VI) Toxic Ions from Water Using Novel Muscovite/Zeolite Aluminosilicate Composite: Adsorption Behavior and Mechanism. Environmental Science and Pollution Research 2020, 27 (12), 13247– 13260,  DOI: 10.1007/s11356-020-07945-8
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    41
    Effective decontamination of As(V), Hg(II), and U(VI) toxic ions from water using novel muscovite/zeolite aluminosilicate composite: adsorption behavior and mechanism
    Salam, Mohamed Abdel; Abukhadra, Mostafa R.; Mostafa, Merna
    Environmental Science and Pollution Research (2020), 27 (12), 13247-13260CODEN: ESPLEC; ISSN:0944-1344. (Springer)
    Muscovite/phillipsitic zeolite was introduced as a novel inorg. composite of stunning adsorption properties. The composite was investigated in the uptake reactions of Hg(II), As(V), and U(VI) as highly toxic water contaminants considering different adsorption factors. The adsorption properties of muscovite/phillipsitic zeolite are highly dependent on the pH values and the best decontamination percentages can be obtained at pH 4, pH 5, and pH 5 for Hg(II), As(V), and U(VI), resp. The kinetic studies demonstrated adsorption equil. for Hg(II), As(V), and U(VI) after 360 min, 300 min, and 360 min, resp. The equil. modeling suggested monolayer uptake for all the metals and represented mainly by the Langmuir model considering both the values of detn. coeff. and chi-squared (χ2). The estd. max. capacities are 117 mg/g (Hg(II)), 122.5 mg/g (As(V)), and 138.5 mg/g (U(VI)) which are higher values than several studied adsorbents. The Dubinin-Radushkevich adsorption energies of Hg(II) (19.4 kJ/mol), As(V) (25.6 kJ/mol), and U(VI) (26.47 kJ/mol) signify chem. adsorption mechanisms and close to the obtained values for the ion-exchange process. Addnl., the composite is of high reusability properties and was applied effectively for five decontamination cycles.
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    Kumar, U.; Bandayopadhyay, M. Sorption of Cadmium from Aqueous Solution Using Pretreated Rice Husk. Bioresour. Technol. 2006, 97 (1), 104– 109,  DOI: 10.1016/j.biortech.2005.02.027
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    Sorption of cadmium from aqueous solution using pretreated rice husk
    Kumar Upendra; Bandyopadhyay Manas
    Bioresource technology (2006), 97 (1), 104-9 ISSN:0960-8524.
    The sorption of Cd(II) from aqueous solution by rice husk, a surplus agricultural byproduct was investigated. Some simple and low-cost chemical modifications resulted in increasing the sorption capacity of raw rice husk (RRH) from 8.58 mg/g to 11.12, 20.24, 16.18 mg/g and reducing the equilibrium time from 10 h of RRH to 2, 4 and 1 h for epichlorohydrin treated rice husk (ERH), NaOH treated rice husk (NRH), sodium bicarbonate treated rice husk (NCRH), respectively. The effect of pH, sorption kinetics and isotherms were studied in batch experiments. Good correlation coefficient was obtained for pseudo second-order kinetic model, which agreed with chemisorption as the rate-limiting mechanism. Sorption isotherm test showed that equilibrium sorption data were better represented by Langmuir model than the Freundlich model. The highly efficient low cost and the rapid uptake of Cd(II) by NCRH indicated that it could be an excellent alternative for the removal of heavy metal by sorption process.
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    Yuan, P.; Tan, D.; Annabi-Bergaya, F.; Yan, W.; Liu, D.; Liu, Z. From Platy Kaolinite to Aluminosilicate Nanoroll via One-Step Delamination of Kaolinite: Effect of the Temperature of Intercalation. Appl. Clay Sci. 2013, 83–84, 68– 76,  DOI: 10.1016/j.clay.2013.08.027
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    43
    From platy kaolinite to aluminosilicate nanoroll via one-step delamination of kaolinite: Effect of the temperature of intercalation
    Yuan, Peng; Tan, Daoyong; Annabi-Bergaya, Faiza; Yan, Wenchang; Liu, Dong; Liu, Zongwen
    Applied Clay Science (2013), 83-84 (), 68-76CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
    Aluminosilicate nanorolls were prepd. using a method of one-step delamination of kaolinite. In this method, cetyltrimethylammonium chloride (CTMACl) was intercalated into the interlayer space of methoxy-modified kaolinite, which resulted in the delamination and rolling of kaolinite layers. The reaction conditions of CTMACl intercalation significantly influenced the formation of nanorolls, as shown by characterizations using X-ray diffraction, electron microscopy, IR spectroscopy, thermal anal., and nitrogen adsorption. Overall, increasing the CTMACl-intercalation temp. helps to promote the transformation from platy kaolinite to nanorolls. The initial kaolinite particles were mostly transformed to nanorolls in the product prepd. at 80 !!!C, whereas considerable kaolinite particles remained untransformed in the product prepd. at 30 !!!C. At 80 !!!C, the obtained sp. surface area (SSA) and the porous vol. (Vpor) values of the nanoroll product are nearly twice the values obtained at 30 !!!C and the tubular structure exhibits higher thermal persistence. The tubular morphol. and the porosity of these nanorolls obtained at 80 !!!C, were largely retained after calcination at 600-800 !!!C. However, a calcination at 900 !!!C led to an obvious distortion of the nanorolls and a decrease in SSA and Vpor values. The obsd. structural changes of the nanorolls under calcination generally resembled that of natural halloysite but occurred at lower temps. because the prepd. nanorolls were of lower structural order with thinner tube walls.
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    Vivas, E. L.; Cho, K. Efficient Adsorptive Removal of Cobalt(II) Ions from Water by Dicalcium Phosphate Dihydrate. Journal of Environmental Management 2021, 283, 111990  DOI: 10.1016/j.jenvman.2021.111990
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    44
    Efficient adsorptive removal of Cobalt(II) ions from water by dicalcium phosphate dihydrate
    Vivas, Eleazer L.; Cho, Kuk
    Journal of Environmental Management (2021), 283 (), 111990CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
    Although the radionuclide 60Co is widely used, its presence in various effluents demands its removal to preclude environmental pollution and detrimental effects on human health. This study investigated the batch adsorption performance of a potential cobalt adsorbent, dicalcium phosphate dihydrate (DCPD), in immobilizing Co2+ from water. The influences of soln. pH, contact time, initial concn., and competing cations were examd. and discussed. Stable cobalt uptake was obsd. at pH 4-8. The sorption kinetics showed a multi-stage uptake profile, implying that several mechanisms are involved in the adsorption process. Microscopy and structural anal. revealed that DCPD decomps. to its anhyd. form during adsorption, which explains the multistep curve over the entire adsorption period. However, the non-apatitic transformation is not exclusive to cobalt uptake. Intraparticle diffusion also contributed to the overall removal kinetics of Co2+ from water. Considering the Sips isotherm model, the max. Co2+ adsorption capacity of DCPD was 441 mg g-1. Cobalt uptake selectivity dropped in the presence of Ca2+ ions, from 1.21 x 104 to 207 mL g-1, indicating DCPD would be more applicable in treating soft 60Co-contaminated waters. Structural anal., elemental mapping, and qual. anal. of solid residues confirmed that ion exchange is involved in the removal of cobalt from aq. solns.
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  45. 45
    El-Zahhar, A. A.; Awwad, N. S. Removal of Malachite Green Dye from Aqueous Solutions Using Organically Modified Hydroxyapatite. Journal of Environmental Chemical Engineering 2016, 4 (1), 633– 638,  DOI: 10.1016/j.jece.2015.12.014
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    45
    Removal of malachite green dye from aqueous solutions using organically modified hydroxyapatite
    El-Zahhar, Adel A.; Awwad, Nasser S.
    Journal of Environmental Chemical Engineering (2016), 4 (1), 633-638CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
    The removal of malachite green dye (MG) from aq. soln. was studied using organically modified hydroxyapatite. Hydroxyapatite (HAP) was organically modified with different concns. of the org. surfactant ethylhexadecyldimethyl ammonium bromide (EHDAB). The modified apatite was characterized using FTIR, XRD and SEM. The modified apatite was studied for removal of MG from aq. soln. and the exptl. parameters were studied. The effect of contact time, adsorbent dose, dye concn. and temp. was studied. The equil. uptake was increased with increasing the initial dye concn. in soln. The exptl. isotherm data were analyzed using Langmuir adsorption isotherm model. The adsorbed amt. of MG onto the modified apatite was found to increase with increasing the adsorbent concn. The max. monolayer adsorption capacity was found to be 188.18 mg/g at 30°C.
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    Zhang, F.; Ma, B.; Jiang, X.; Ji, Y. Dual Function Magnetic Hydroxyapatite Nanopowder for Removal of Malachite Green and Congo Red from Aqueous Solution. Powder Technol. 2016, 302, 207– 214,  DOI: 10.1016/j.powtec.2016.08.044
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    Dual function magnetic hydroxyapatite nanopowder for removal of malachite green and Congo red from aqueous solution
    Zhang, Fan; Ma, Baoliang; Jiang, Xiping; Ji, Yuefei
    Powder Technology (2016), 302 (), 207-214CODEN: POTEBX; ISSN:0032-5910. (Elsevier B.V.)
    In this study, the removal of both cationic dye (malachite green) and anionic dye (Congo red) by magnetic Sr5xBa3x(PO4)3(OH)/Fe3O4 nanopowder (namely SBPF) from aq. soln. was investigated. Variables influencing the adsorption capacity, such as soln. pH, temp., adsorbent dosage, adsorption time, and initial concn., were systematically investigated. The adsorption process is pH and temp. dependent. The adsorption for MG and CR can be described by pseudo-first-order and pseudo-second-order kinetic model, resp. The adsorption behaviors fit quite well with the Langmuir model for both dyes with the max. adsorption capacity of 526 mg g-1 for MG and 417 mg g-1 for CR. Thermodn. anal. revealed that the adsorption processes were spontaneous and exothermic. Phys. forces, hydrogen bonding, and ionic interaction are responsible for binding of the dyes with SBPF. The used SBPF nanopowder could be regenerated effectively and recycled for five cycles without a significant loss of adsorption ability. Moreover, the adsorbent can be applied to remove MG and CR in different water matrixes.
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    Lee, Y.-C.; Kim, J.-Y.; Shin, H.-J. Removal of Malachite Green (MG) From Aqueous Solutions by Adsorption, Precipitation, and Alkaline Fading Using Talc. Sep. Sci. Technol. 2013, 48 (7), 1093– 1101,  DOI: 10.1080/01496395.2012.723100
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    47
    Removal of Malachite Green (MG) From Aqueous Solutions by Adsorption, Precipitation, and Alkaline Fading Using Talc
    Lee, Young-Chul; Kim, Jin-Young; Shin, Hyun-Jae
    Separation Science and Technology (Philadelphia, PA, United States) (2013), 48 (7), 1093-1101CODEN: SSTEDS; ISSN:0149-6395. (Taylor & Francis, Inc.)
    Malachite Green (MG), which is primarily used as a dye, is a chem. that is listed as a class II health hazard because of its toxicity to humans and the environment. Adsorption is frequently used to remove this cationic dye from aq. solns. Structural changes of the mol. should be considered during removal, because MG (or chromatic MG+ at neutral pH) turns into protonated MG (MGH+) at acidic pHs and a carbinol base at basic pHs. Batch sorption expts. were conducted to remove MG from aq. solns. using talc. We studied specific removal behaviors and mechanisms of the MG for different pH solns., including adsorption, pptn., and alk. fading.
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    Chen, Y.; Nie, Z.; Gao, J.; Wang, J.; Cai, M. A Novel Adsorbent of Bentonite Modified Chitosan-Microcrystalline Cellulose Aerogel Prepared by Bidirectional Regeneration Strategy for Pb(II) Removal. Journal of Environmental Chemical Engineering 2021, 9 (4), 105755  DOI: 10.1016/j.jece.2021.105755
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    48
    A novel adsorbent of bentonite modified chitosan-microcrystalline cellulose aerogel prepared by bidirectional regeneration strategy for Pb(II) removal
    Chen, Yan; Nie, Zeguang; Gao, Junkai; Wang, Jiaqi; Cai, Miaomiao
    Journal of Environmental Chemical Engineering (2021), 9 (4), 105755CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
    Traditional chitosan aerogel (CSA) could be used to chelate heavy metal ions due to its large sp. surface area, high porosity and rich amino groups. However, the CSA was rarely applied in practical application because of its easy hydrolysis, low mech. strength and slow adsorption rate. In this study, we developed a novel method for increasing the anti-hydrolytic ability and mech. strength of CSA by bidirectional regeneration of chitosan and microcryst. cellulose to synthesize chitosan-microcryst. cellulose aerogel (CS-MCCA). In addn., bentonite (BT) was introduced in the regeneration process to enhance the adsorption rate of CSA, and an efficient adsorbent of bentonite-chitosan-microcryst. cellulose aerogel (BT-CS-MCCA) for Pb(II) removal was developed, and the max. adsorption amt. and adsorption equil. time of Pb(II) on BT-CS-MCCA were 256.24 mg g-1 and 60 min, resp. Addnl., it was found that with the increase of Na+ or K+ concn. in the soln. from 0 mol L-1 to 0.1 mol L-1, the adsorption capacity of BT-CS-MCCA was enhanced, because the Ca2+ in BT was substituted by Na+ or K+ , and then the ion-exchange ability of BT-CS-MCCA was improved. Moreover, the prepn. method of BT-CS-MCCA possessed merits of simple operation, low cost and hypotoxicity. Thus, the BT-CS-MCCA had a broad potential application for the purifn. of Pb(II) in wastewater, and the bidirectional regeneration strategy might offer a brand-new path for the utilization of biomass resources.
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    Tran, T. N.; Do, Q. C.; Kim, D.; Kim, J.; Kang, S. Urchin-like Structured Magnetic Hydroxyapatite for the Selective Separation of Cerium Ions from Aqueous Solutions. Journal of Hazardous Materials 2022, 430, 128488  DOI: 10.1016/j.jhazmat.2022.128488
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    Urchin-like structured magnetic hydroxyapatite for the selective separation of cerium ions from aqueous solutions
    Tran, Thi Nhung; Do, Quoc Cuong; Kim, Dogun; Kim, Junho; Kang, Seoktae
    Journal of Hazardous Materials (2022), 430 (), 128488CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
    In this study, bio-inspired urchin-like structured hydroxyapatite (UHdA) and its magnetic composite (UHdA@Fe3O4) were developed for efficient and easy sepn. of cerium ions (Ce3+) from aquatic waste streams. UHdA and UHdA@Fe3O4 exhibited superior Ce3+ adsorption capacities of 248.39 and 230.01 mg/g-UHdA resp., compared to a com. HdA (141.71 mg/g-HdA) due to their hierarchical mesoporous structure and large sp. surface area. The adsorption of Ce3+ to UHdA and UHdA@Fe3O4 were heterogeneous, pseudo-second-order-kinetic, and the rate-limiting step was external mass transfer and intra-particle diffusion. Moreover, thermodn. studies revealed that the adsorption process was spontaneous and endothermic nature. The high selectivity towards Ce3+ in multi-ionic systems is attributed to the strong affinity between strong Lewis acid (Ce3+) and base (PO3-4 and OH-) interactions. XRD, FTIR, and XPS anal. demonstrated that the adsorption was mainly attributable to the ion exchange of Ce3+ with Ca2+ and to surface complexation. The desorption of Ce3+ was efficiently accomplished using 0.1 M HNO3. The results suggest that UHdA and UHdA@Fe3O4 could be promising choices for the adsorption and recovery of rare earth elements.
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    El Qada, E. Kinetic Behavior of the Adsorption of Malachite Green UsingJordanian Diatomite as Adsorbent. JORDANIAN JOURNAL OF ENGINEERING AND CHEMICAL INDUSTRIES (JJECI) 2020, 3 (1), 1– 10,  DOI: 10.48103/jjeci3120220
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    Lin, X.; Xie, Y.; Lu, H.; Xin, Y.; Altaf, R.; Zhu, S.; Liu, D. Facile Preparation of Dual La-Zr Modified Magnetite Adsorbents for Efficient and Selective Phosphorus Recovery. Chemical Engineering Journal 2021, 413, 127530  DOI: 10.1016/j.cej.2020.127530
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    Facile preparation of dual La-Zr modified magnetite adsorbents for efficient and selective phosphorus recovery
    Lin, Xiaochang; Xie, Yinglong; Lu, Huijie; Xin, Yicong; Altaf, Rubina; Zhu, Songming; Liu, Dezhao
    Chemical Engineering Journal (Amsterdam, Netherlands) (2021), 413 (), 127530CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
    Phosphate (P) is an irreplaceable resource for the growth of all living organisms, and the impending exhaustion of minable P rock arouses the demand of P recovery, which further promotes the novel technologies development. To reclaim the P from wastewater or sludge conveniently and efficiently, a novel magnetic adsorbent with La-Zr bimetallic modification (La-Zr@Fe3O4) possessing a high affinity to phosphate and rapid sepn. was proposed in this study. Adsorption tests showed that the adsorption capacity of P on La-Zr@Fe3O4 increased with La content, reaching the max. value of 49.3 mg/g at pH 3 by L1Z2. Whereas, the addn. of La resulted in the decline of desorption efficiency from ∼85% to ∼60% in the pH range from 3 to 6, except pH 2. The kinetics of P adsorption on the La-Zr@Fe3O4 was described well by the pseudo-second-order model, while the isotherm of P adsorption was fitted well by the Freundlich model. Besides, the adsorbent exhibited high selectivity towards P over other coexisting ions (Cl-, NO-3, SO2-4, Mg2+, and Ca2+). The feasibility of P recovery from the solid phase was investigated and confirmed by P recovery from fish farm sludge. The 90% removal efficiency of P and 88% desorption efficiency in cyclic adsorption/desorption expts. evidenced the stability and reusability of La-Zr magnetic adsorbent. The anal. of X-ray diffraction, Fourier transform IR spectrum, and XPS revealed the replacement of OH- with phosphate via the ligand exchange was the adsorption mechanism. This work demonstrated that the highly efficient, rapidly separable, and repeatable La-Zr@Fe3O4 has the potential for phosphate sequestration and recovery.
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    Jiang, Y.; Abukhadra, M. R.; Refay, N. M.; Sharaf, M. F.; El-Meligy, M. A.; Awwad, E. M. Synthesis of Chitosan/MCM-48 and β-Cyclodextrin/MCM-48 Composites as Bio-Adsorbents for Environmental Removal of Cd2+ Ions; Kinetic and Equilibrium Studies. React. Funct. Polym. 2020, 154, 104675  DOI: 10.1016/j.reactfunctpolym.2020.104675
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    Synthesis of chitosan/MCM-48 and β-cyclodextrin/MCM-48 composites as bio-adsorbents for environmental removal of Cd2+ ions; kinetic and equilibrium studies
    Jiang, Yuliang; Abukhadra, Mostafa R.; Refay, Nermen M.; Sharaf, Mohamed F.; El-Meligy, Mohammed A.; Awwad, Emad Mahrous
    Reactive & Functional Polymers (2020), 154 (), 104675CODEN: RFPOF6; ISSN:1381-5148. (Elsevier Ltd.)
    Chitosan/MCM-48 (CH/MCM) and β-cyclodextrin/MCM-48 (CD/MCM) composites were synthesized as promising and eco-friendly bio-adsorbents for Cd2+ ions from water. The composites showed novel porous structures and complex functional groups making them of high adsorption capacities. The adsorption behaviors of CH/MCM and CD/MCM are highly controlled by the tested pH values realizing their best capacities at pH 7. The kinetic evaluation indicated the excellent agreement between the uptake of Cd2+ by CH/MCM and CD/MCM with the pseudo-first-order model achieving equil. intervals of 480 min and 600 min, resp. Based on the values of Chi-squared (X2) and the correlation coeff., the composites displayed adsorption properties related to the Freundlich hypothesis with a multilayer form. Addnl., the Gaussian energies of them are 2.23 KJ/mol (CH/MCM) and 2.46 KJ/mol (CD/MCM) reflecting phys. uptake of Cd2+ by the studied composites. The thermodn. investigation implied spontaneous uptake of Cd2+ by the composites with endothermic reactions. The prepd. CH/MCM and CD/MCM are of 122.4 mg/g and 152.2 mg/g theor. qmax, resp. which are higher values than the reported results for several studied adsorbents. Moreover, the synthetic CH/MCM and CD/MCM showed high reusability as adsorbents for Cd2+ to be applied effectively six times.
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    Sherlala, A. I. A.; Raman, A. A. A.; Bello, M. M.; Buthiyappan, A. Adsorption of Arsenic Using Chitosan Magnetic Graphene Oxide Nanocomposite. Journal of Environmental Management 2019, 246, 547– 556,  DOI: 10.1016/j.jenvman.2019.05.117
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    Adsorption of arsenic using chitosan magnetic graphene oxide nanocomposite
    Sherlala, A. I. A.; Raman, A. A. A.; Bello, M. M.; Buthiyappan, A.
    Journal of Environmental Management (2019), 246 (), 547-556CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
    Chitosan-magnetic-graphene oxide (CMGO) nanocomposite was prepd. for arsenic adsorption. The nanocomposite was characterized through BET, FTIR, FESEM, EDX, and VSM analyses. These characterizations confirmed the formation of CMGO nanocomposites with high sp. surface area (152.38 m2/g) and excellent satn. magnetization (49.30 emu/g). Batch adsorption expts. were conducted to evaluate the performance of the nanocomposite in the adsorption of arsenic from aq. soln. The effects of operational parameters, adsorption kinetic, equil. isotherm and thermodn. were evaluated. The removal efficiency of arsenic increased with increasing adsorbent dosage and contact time. However, the effect of pH followed a different pattern, with the removal efficiency increasing from acidic to neutral pH, and then decreasing at alk. conditions. The highest adsorption capacity (45 mg/g) and removal efficiency (61%) were obtained at pH 7.3. The adsorption kinetic followed a pseudo-second-order kinetic model. The anal. of adsorption isotherm shows that the adsorption data fitted well to Langmuir isotherm model, indicating a homogeneous process. Thermodn. anal. shows that the adsorption of As(III) is exothermic and spontaneous. The superparamagnetic properties of the nanocomposite enabled the sepn. and recovery of the nanoparticles using an external magnetic field. Thus, the developed nanocomposite has a potential for arsenic remediation.
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    Huang, Y.; Zeng, X.; Guo, L.; Lan, J.; Zhang, L.; Cao, D. Heavy Metal Ion Removal of Wastewater by Zeolite-Imidazolate Frameworks. Sep. Purif. Technol. 2018, 194, 462– 469,  DOI: 10.1016/j.seppur.2017.11.068
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    Heavy metal ion removal of wastewater by zeolite-imidazolate frameworks
    Huang, Yan; Zeng, Xiaofei; Guo, Lingling; Lan, Jianhui; Zhang, Liangliang; Cao, Dapeng
    Separation and Purification Technology (2018), 194 (), 462-469CODEN: SPUTFP; ISSN:1383-5866. (Elsevier B.V.)
    With the rapid development of industrialization, removing heavy metal ions of wastewater from the discharge of industrial sewage is a very important topic, because it will severely affect our environment and water ecosystem. In this work, we synthesize two porous adsorbents of ZIF-8 and ZIF-67 and further investigate their performance of removing Pb2+ and Cu2+ from wastewater. Results indicate that satd. adsorption capacities of ZIF-8 and ZIF-67 for Pb2+ reach 1119.80 and 1348.42 mg/g, while they are 454.72 and 617.51 mg/g for Cu2+, resp., which are greatly higher than almost all other porous materials. If we use the excessive adsorbents to treat wastewater, more than 99.4% Pb2+ and 97.4% Cu2+ can be removed by ZIF-8 and ZIF-67 adsorbents. Moreover, the two adsorbents also show fast adsorption kinetics, and only need several decade minutes to reach adsorption equil. These features indicate that ZIF-8 and ZIF-67 are excellent candidates for removal of heavy metal ions from wastewater.
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    Jasper, E. E.; Ajibola, V. O.; Onwuka, J. C. Nonlinear Regression Analysis of the Sorption of Crystal Violet and Methylene Blue from Aqueous Solutions onto an Agro-Waste Derived Activated Carbon. Appl. Water Sci. 2020, 10 (6), 132,  DOI: 10.1007/s13201-020-01218-y
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    Nonlinear regression analysis of the sorption of crystal violet and methylene blue from aqueous solutions onto an agro-waste derived activated carbon
    Jasper, Enebi Estella; Ajibola, Victor Olatunji; Onwuka, Jude Chinedu
    Applied Water Science (2020), 10 (6), 132CODEN: AWSPCL; ISSN:2190-5495. (Springer GmbH)
    Abstr.: Sorption of synthetic dyes on low-cost solid sorbents is a simple technique for their removal from wastewater. This research investigates the sorption kinetics and equil. of two synthetic cationic dyes, crystal violet and methylene blue from aq. media using activated carbon prepd. from an agro-waste, Millettia thonningii seed pods. Sorption expts. were carried out using the batch process. The kinetic data were analyzed using the pseudo-first-order, pseudo-second-order, and intraparticle diffusion models while the equil. data were analyzed using the Langmuir, Freundlich, and Redlich-Peterson isotherm models. Nonlinear regression method was used to fit the data to the isotherm models in order to det. model parameters and the best-fit isotherms. Thus, three error functions; coeff. of detn., Chi-square statistic test, and the sum of error squares were applied to evaluate the sorption data. The pseudo-second-order model best described the sorption kinetics of both dyes while the Redlich-Peterson model described the equil. data the most, followed closely by the Freundlich isotherm model indicating a heterogeneous sorbent surface. The exptl. results indicate that the agro-waste derived activated carbon is a viable adsorbent for the remediation of dye-contaminated water.
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    Giles, C. H.; MacEwan, T. H.; Nakhwa, S. N.; Smith, D. 786. Studies in Adsorption. Part XI. A System of Classification of Solution Adsorption Isotherms, and Its Use in Diagnosis of Adsorption Mechanisms and in Measurement of Specific Surface Areas of Solids. Journal of the Chemical Society (Resumed) 1960, 3973,  DOI: 10.1039/jr9600003973
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    Abukhadra, M. R.; Dardir, F. M.; Shaban, M.; Ahmed, E. A.; Soliman, M. F. Superior Removal of Co2+, Cu2+ and Zn2+ Contaminants from Water Utilizing Spongy Ni/Fe Carbonate–Fluorapatite; Preparation, Application and Mechanism. Ecotoxicology and Environmental Safety 2018, 157, 358– 368,  DOI: 10.1016/j.ecoenv.2018.03.085
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    Superior removal of Co2+, Cu2+ and Zn2+ contaminants from water utilizing spongy Ni/Fe carbonate-fluorapatite; preparation, application and mechanism
    Abukhadra, Mostafa R.; Dardir, Fatma M.; Shaban, Mohamed; Ahmed, Ezzat A.; Soliman, Mamdouh F.
    Ecotoxicology and Environmental Safety (2018), 157 (), 358-368CODEN: EESADV; ISSN:0147-6513. (Elsevier B.V.)
    Spongy Ni/Fe carbonate - fluorapatite was synthesized from natural phosphorite enriched with iron impurities. The morphol., chem. and structural features of the product were estd. using several techniques as XRD, SEM, EDX, and FT-IR. It exhibits spongy structure of nano and micro-pores. The av. crystallite size is about 8.27nm. The suitability of the product for considerable decontamination of Zn2+, Co2+, and Cu2+, ions from water was studied based on several reacting parameters. The equil. was attained after 240min for Zn2+ and Co2+ ions while the adsorption equil. of Cu2+ reached after 120min. The adsorption data for the selected metals was represented well by a pseudo-second-order model which revealed chemisorption uptake. The equil. studies were appraised based on traditional models and two advanced models were designed according to the statistical phys. theories. The adsorption results highly fitted with Langmuir model followed rather than the other models. This indicated a monolayer adsorption for the metal ions by spongy Ni/Fe carbonate - fluorapatite. The estd. qmax values are 149.25mg/g, 106.4mg/g and 147.5mg/g for the uptake of Zn2+, Co2+, and Cu2+, resp. Based on monolayer models of one energy and two energies, the no. of receptor adsorption sites, no. of adsorbed metal ions per active site, the av. no. of sites which occupied by ions, mono layer adsorption quantity and the adsorption quantity after total satn. were calcd. for the first time for such materials.
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    Shaban, M.; Abukhadra, M. R.; Shahien, M. G.; Khan, A. A. P. Upgraded Modified Forms of Bituminous Coal for the Removal of Safranin-T Dye from Aqueous Solution. Environmental Science and Pollution Research 2017, 24 (22), 18135– 18151,  DOI: 10.1007/s11356-017-9424-4
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    Upgraded modified forms of bituminous coal for the removal of safranin-T dye from aqueous solution
    Shaban, Mohamed; Abukhadra, Mostafa R.; Shahien, Mohamed G.; Khan, Aftab Aslam Parwaz
    Environmental Science and Pollution Research (2017), 24 (22), 18135-18151CODEN: ESPLEC; ISSN:0944-1344. (Springer)
    Natural bituminous coal was used as a precursor in the synthesis of different modified products. The modification of coal was performed by treating it with nitric acid (N-coal), coating its surface by zinc oxide nanoparticles (Z-coal), and converting it into porous graphite (PG). The effect of modification processes on the structures, morphologies, and optical properties was followed by X-ray diffraction (XRD), SEM (SEM), Fourier transform IR spectrum (FT-IR), and UV/VIS spectrophotometer anal. The surface of N-coal grains becomes smoother than the surface of raw coal grains due to the removal of the assocd. impurities and the formation of nitrogen function groups. For Z-coal, the whole surface of coal grains appears to be completely covered by agglomerated ZnO nanoparticles of massive d. and irregular shapes. The av. crystallite size of the formed ZnO is ∼22.2 nm and d. of dislocations is 2.029 × 10-3 dislocation/nm2. Also, the removal of safranin-T dye by natural bituminous coal and its modified forms was investigated as a function of contact time, adsorbent mass, initial dye concn., and pH value. The obtained results are well fitted by pseudo-second-order kinetic than by intraparticle diffusion and Elovich kinetic models for the adsorption by N-coal, Z-coal, and PG, whereas the adsorption by raw coal is well fitted with both pseudo-second-order and Elovich kinetic models.
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    Faisal, M. L. F. M. Batch Sorption of Copper (II) Ions from Simulated Aqueous Solution by Banana Peel. Al-Khwarizmi Eng. J. 2017, 12 (4), 117– 125,  DOI: 10.22153/kej.2016.05.004
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    Mobarak, M.; Ali, R. A. M.; Seliem, M. K. Chitosan/Activated Coal Composite as an Effective Adsorbent for Mn(VII): Modeling and Interpretation of Physicochemical Parameters. Int. J. Biol. Macromol. 2021, 186, 750– 758,  DOI: 10.1016/j.ijbiomac.2021.07.089
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    Chitosan/activated coal composite as an effective adsorbent for Mn(VII): Modeling and interpretation of physicochemical parameters
    Mobarak, Mohamed; Ali, Rabea A. M.; Seliem, Moaaz K.
    International Journal of Biological Macromolecules (2021), 186 (), 750-758CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    Chitosan was impregnated into porous activated coal to produce a multifunctional chitosan/activated coal (Cs/Ac) composite. The resulted Cs/Ac was characterized and utilized as a cost-effective adsorbent for Mn(VII) at altered temps. (i.e., 25, 35, and 45°C). The adsorption results were fitted to classical as well as advanced statistical physics models. The Freundlich equation described well the achieved exptl. data at all temps. Enhancing the Langmuir adsorption capacity from 203.26 to 224.03 mg/g with temp. indicated that Mn(VII) adsorption was an endothermic process. Steric, energetic and thermodn. data of the double layer model with two energy sites (i.e., the best fit statistical model) were completely interpreted. The no. of Mn(VII) per adsorption site (n) was between 0.76 and 0.92 suggested the presence of multi-docking and multi-interactions mechanisms. The active sites d. (NM) of the Cs/Ac decreased with improving temp. Energetically, Mn(VII) uptake by Cs/Ac was governed by phys. interactions (i.e., adsorption energy <40 kJ/mol). Macroscopically, the interaction between Mn(VII) and Cs/Ac was spontaneous. Overall, modification of the Ac by the used marine biomass (Cs) produced a promising Mn(VII) adsorbent and also, the application of phys. anal. offered a deep interpretation for the adsorption mechanism.
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  61. 61
    Ashraf, M.-T.; AlHammadi, A. A.; El-Sherbeeny, A. M.; Alhammadi, S.; Al Zoubi, W.; Ko, Y. G.; Abukhadra, M. R. Synthesis of Cellulose Fibers/Zeolite-A Nanocomposite as an Environmental Adsorbent for Organic and Inorganic Selenium Ions; Characterization and Advanced Equilibrium Studies. J. Mol. Liq. 2022, 360, 119573  DOI: 10.1016/j.molliq.2022.119573
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    Synthesis of cellulose fibers/Zeolite-A nanocomposite as an environmental adsorbent for organic and inorganic selenium ions; Characterization and advanced equilibrium studies
    Ashraf, Menna-Tullah; AlHammadi, Ali A.; El-Sherbeeny, Ahmed M.; Alhammadi, Salh; Al Zoubi, Wail; Ko, Young Gun; Abukhadra, Mostafa R.
    Journal of Molecular Liquids (2022), 360 (), 119573CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
    Cellulose fibers/Zeolite-A composite (CF/ZA) was synthesized as an innovative hybrid structure of enhanced adsorption properties for different selenium species (inorg. (selenate (Se VI)), selenite (Se (IV)), and org. (selenomethionine (SeMt)). The CF/ZA composite achieved actual adsorption capacities of 163 mg/g (Se (VI)), 212.4 mg/g (Se (IV)), and 109.3 mg/g (SeMt) which are higher values than zeolite, cellulose, and several studied adsorbents in literature. The kinetic and classic equil. studies are in agreement with Pseudo-First order kinetics (R2 > 0.95) and Langmuir isotherm (R2 > 0.89). This suggests homogenous, monolayer, and more phys. uptake of the three selenium species. The monolayer model of one energy was assessed as an advanced equil. model. Based on the steric n parameter (2.88-3.31(Se (VI), 2.22-5.94 (Se (IV), and 3.46-4.41 (SeMt)) demonstrate the adsorption of them as three or more ions per each site in a vertical orientation by multi-ionic mechanisms. The adsorption energies (-20.78 to -27.14 kJ/mol) are related to physisorption processes such as hydrogen bonding (<30 kJ/mol) and dipole bonding forces (2-29 kJ/mol). The Gaussian energies (1.04-2.09 kJ/mol) support the physisorption reactions in addn. to zeolitic ion exchange processes. The thermodn. functions (internal energy, free enthalpy, and entropy) demonstrate the exothermic, feasible, and spontaneous properties of the reactions.
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  62. 62
    Dhaouadi, F.; Sellaoui, L.; Reynel-Ávila, H. E.; Landín-Sandoval, V.; Mendoza-Castillo, D. I.; Jaime-Leal, J. E.; Lima, E. C.; Bonilla-Petriciolet, A.; Lamine, A. B. Adsorption Mechanism of Zn2+, Ni2+, Cd2+, and Cu2+ Ions by Carbon-Based Adsorbents: Interpretation of the Adsorption Isotherms via Physical Modelling. Environmental Science and Pollution Research 2021, 28 (24), 30943– 30954,  DOI: 10.1007/s11356-021-12832-x
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    Adsorption mechanism of Zn2+, Ni2+, Cd2+, and Cu2+ ions by carbon-based adsorbents: interpretation of the adsorption isotherms via physical modelling
    Dhaouadi, Fatma; Sellaoui, Lotfi; Reynel-Avila, Hilda Elizabeth; Landin-Sandoval, Veronica; Mendoza-Castillo, Didilia I.; Jaime-Leal, Jose Enrique; Lima, Eder Claudio; Bonilla-Petriciolet, Adrian; Lamine, Abdelmottaleb Ben
    Environmental Science and Pollution Research (2021), 28 (24), 30943-30954CODEN: ESPLEC; ISSN:0944-1344. (Springer)
    A theor. physicochem. and thermodn. investigation of the adsorption of heavy metals Zn2+, Cd2+, Ni2+, and Cu2+ on carbon-based adsorbents was performed with statistical physics fundaments. Particularly, the exptl. adsorption isotherms of heavy metal removal, at 30°C and pH 5, using adsorbents obtained from the pyrolysis of three biomasses (cauliflower cores, broccoli stalks, and coconut shell) were modelled and interpreted with a homogeneous statistical physics adsorption model. Calcns. indicated that the heavy metal adsorption with these carbon-based materials was a multi-ionic process where several ions interact simultaneously with the same carboxylic functional group on the adsorbent surface. Adsorption capacities for these metal ions and adsorbents were correlated with electronegativity theory, which established that the adsorbate with the highest electronegativity was more readily adsorbed by the carboxylic functional groups available on the adsorbent surfaces. Also, the chem. compns. of biomass precursors explained achieved adsorption capacities for these metallic ions. The best adsorbent for heavy metal removal was obtained from CC biomass pyrolysis. Calcd. adsorption energies for heavy metal removal could be assocd. with physisorption-type forces. Finally, the adsorption mechanism anal. was complemented with the detn. of adsorption thermodn. functions using the statistical physics.
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  63. 63
    Sellaoui, L.; Ali, J.; Badawi, M.; Bonilla-Petriciolet, A.; Chen, Z. Understanding the Adsorption Mechanism of Ag+ and Hg2+ on Functionalized Layered Double Hydroxide via Statistical Physics Modeling. Appl. Clay Sci. 2020, 198, 105828  DOI: 10.1016/j.clay.2020.105828
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    Understanding the adsorption mechanism of Ag+ and Hg2+ on functionalized layered double hydroxide via statistical physics modeling
    Sellaoui, Lotfi; Ali, Jawad; Badawi, Michael; Bonilla-Petriciolet, Adrian; Chen, Zhuqi
    Applied Clay Science (2020), 198 (), 105828CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
    Modeling anal. based on a statistical physics theory was used to explain the adsorption of Ag+ and Hg2+ on layered double hydroxides (LDH) functionalized with anions CO32-, NO3-, S52- and MoS42-. Theor. adsorption models assuming different types of functional groups on LDH surface were tested and compared. A statistical physics model based on two active sites for the adsorbate binding was the best option to characterize and interpret the removal of investigated heavy metals on LDH. Modeling results showed that the total adsorption capacities at satn. ranged from 112 to 631 mg/g and from 110 to 638 mg/g for Ag+ and Hg2+, resp. LDH functionalized with anion MoS2-4 was the best adsorbent for the removal of both metal ions. It was also demonstrated that the anionic functionalities and the oxygen-contg. groups of LDH contributed in different extent for the adsorption of Ag+ and Hg2+. Statistical physics parameters suggested a multi-ionic and endothermic adsorption caused by phys. and chem. interactions. Finally, the adsorption mechanism was macroscopically explained via the calcn. and anal. of thermodn. potentials.
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  64. 64
    Ali, R. A. M.; Mobarak, M.; Badawy, A. M.; Lima, E. C.; Seliem, M. K.; Ramadan, H. S. New Insights into the Surface Oxidation Role in Enhancing Congo Red Dye Uptake by Egyptian Ilmenite Ore: Experiments and Physicochemical Interpretations. Surfaces and Interfaces 2021, 26, 101316  DOI: 10.1016/j.surfin.2021.101316
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    64
    New insights into the surface oxidation role in enhancing Congo red dye uptake by Egyptian ilmenite ore: Experiments and physicochemical interpretations
    Ali, Rabea A. M.; Mobarak, Mohamed; Badawy, Aliaa M.; Lima, Eder C.; Seliem, Moaaz K.; Ramadan, H. S.
    Surfaces and Interfaces (2021), 26 (), 101316CODEN: SIUNCN; ISSN:2468-0230. (Elsevier B.V.)
    The continuous discharge of org. dyes into the aquatic environment represents a main reason for water contamination. Removal of dye mols. via adsorption is suggested to be an effective, simple, and low-cost technol. Herein, two representative samples of black ilmenite and its oxidized red form were characterized and tested as adsorbents for Congo red (CR) dye. The high concns. of iron-titanium oxides in the red ilmenite was due to the surface alteration. The red ilmenite displayed high adsorption capacities against CR compared to the black one at varied pH values (i.e. 5.0-9.0). The Freundlich model described well the CR data at all adsorption temps. (25, 40, and 50°C). The physicochem. parameters of the multilayer model were employed to recognize the interface mechanisms between CR mols. and the ilmenite active sites. The values of receptor sites (n) ranged from 0.60 to 0.91 (i.e., n < 1.0 at all temps.) suggesting a horizontal position and multi-docking adsorption mechanism. In the temp. range of 25-50°C, the increase of the total removed CR layers (the Nt parameter) from 2.9 to 4.4 resulted in enhancing the adsorption capacity at satn. (Qsat) from 158.23 to 267.96 mg/g. The values of adsorption energies varied from 13.26 to 18.356 kJ/mol reflected that CR adsorption onto the RI was endothermic and assocd. to phys. interactions. Overall, the high performance of the red ilmenite was mainly assocd. with the control of surface alteration. Furthermore, utilizing the multilayer statistical model described the interaction mechanism between CR and ilmenite adsorption sites at mol. level.
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  65. 65
    Dhaouadi, F.; Sellaoui, L.; Badawi, M.; Reynel-Ávila, H. E.; Mendoza-Castillo, D. I.; Jaime-Leal, J. E.; Bonilla-Petriciolet, A.; Lamine, A. B. Statistical Physics Interpretation of the Adsorption Mechanism of Pb2+, Cd2+ and Ni2+ on Chicken Feathers. J. Mol. Liq. 2020, 319, 114168  DOI: 10.1016/j.molliq.2020.114168
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    65
    Statistical physics interpretation of the adsorption mechanism of Pb2+, Cd2+ and Ni2+ on chicken feathers
    Dhaouadi, Fatma; Sellaoui, Lotfi; Badawi, Michael; Reynel-Avila, Hilda Elizabeth; Mendoza-Castillo, Didilia Ileana; Jaime-Leal, Jose Enrique; Bonilla-Petriciolet, Adrian; Lamine, Abdelmottaleb Ben
    Journal of Molecular Liquids (2020), 319 (), 114168CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
    The mechanism of adsorption of Pb2+, Cd2+ and Ni2+ on chicken feathers was studied via statistical physics theory. A detailed theor. anal. was performed using three models that assumed the adsorption of these metal ions via one, two or three types of surface functionalities from chicken feathers. These surface functionalities corresponded to carboxylic, disulfide and amino groups. The monolayer adsorption model with two types of functional groups was selected to analyze the steric and energetic factors involved in the removal of these heavy metals. Results of the statistical physics modeling showed that this adsorption system was multi-ionic with the presence of both endothermic and exothermic adsorption stages depending on soln. temp. Calcd. adsorption energies were assocd. to phys. adsorption forces where the carboxylic and disulfide functional groups were responsible of metal binding on chicken feathers. Thermodn. calcns. of configuration entropy, free enthalpy and internal energy indicated that the adsorption of Pb2+, Cd2+ and Ni2+ on chicken feathers was a spontaneous and feasible process. These findings contribute to understand and characterize the thermodn. nature of the adsorption of heavy metal ions on natural adsorbents like chicken feathers.
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  66. 66
    Shemy, M. H.; Othman, S. I.; Alfassam, H. E.; Al-Waili, M. A.; Alqhtani, H. A.; Allam, A. A.; Abukhadra, M. R. Synthesis of Green Magnetite/Carbonized Coffee Composite from Natural Pyrite for Effective Decontamination of Congo Red Dye: Steric, Synergetic, Oxidation, and Ecotoxicity Studies. Catalysts 2023, 13 (2), 264,  DOI: 10.3390/catal13020264
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    66
    Synthesis of Green Magnetite/Carbonized Coffee Composite from Natural Pyrite for Effective Decontamination of Congo Red Dye: Steric, Synergetic, Oxidation, and Ecotoxicity Studies
    Shemy, Marwa H.; Othman, Sarah I.; Alfassam, Haifa E.; Al-Waili, Maha A.; Alqhtani, Haifa A.; Allam, Ahmed A.; Abukhadra, Mostafa R.
    Catalysts (2023), 13 (2), 264CODEN: CATACJ; ISSN:2073-4344. (MDPI AG)
    Green magnetite/carbonized spent coffee (MG/CFC) composite was synthesized from natural pyrite and characterized as an adsorbent and catalyst in photo-Fenton's oxidn. system of Congo red dye (C.R). The absorption behavior was illustrated based on the steric and energetic parameters of the advanced Monolayer equil. model of one energetic site (R2 > 0.99). The structure exhibits 855 mg/g as effective site d. which induces its C.R satn. adsorption capacity to 436.1 mg/g. The change in the no. of absorbed C.R per site with temp. (n = 1.53 (293) to 0.51 (313 K)) suggests changes in the mechanism from multimol. (up to 2 mols. per site) to multianchorage (one mol. per more than one site) processes. The energetic studies (ΔE = 6.2-8.2 kJ/mol) validate the phys. uptake of C.R by MG/CFC which might be included van der Waals forces, electrostatic attractions, and hydrogen bonding. As a catalyst, MG/CFC exhibits significant activity during the photo-Fenton's oxidn. of C.R under visible light. The complete oxidn. of C.R was detected after 105 min (5 mg/L), 120 min (10 mg/L), 135 min (15 mg/L), 180 min (20 mg/L), and 240 min (25 mg/L) using MG/CFC at 0.2 g/L dosage and 0.1 mL of H2O2. Increasing the dosage up to 0.5 g/L reduce the complete oxidn. interval of C.R (5 mg/L) down to 30 min while the complete mineralization was detected after 120 min. The acute and chronic toxicities of the treated samples demonstrate significant safe products of no toxic effects on aquatic organisms as compared to the parent C.R soln.
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  67. 67
    Sellaoui, L.; Guedidi, H.; SarraWjihi, S.; Reinert, L.; Knani, S.; Duclaux, L.; Ben Lamine, A. Experimental and Theoretical Studies of Adsorption of Ibuprofen on Raw and Two Chemically Modified Activated Carbons: New Physicochemical Interpretations. RSC Adv. 2016, 6 (15), 12363– 12373,  DOI: 10.1039/C5RA22302D
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    67
    Experimental and theoretical studies of adsorption of ibuprofen on raw and two chemically modified activated carbons: new physicochemical interpretations
    Sellaoui, Lotfi; Guedidi, Hanen; SarraWjihi; Reinert, Laurence; Knani, Salah; Duclaux, Laurent; Ben Lamine, Abdelmottaleb
    RSC Advances (2016), 6 (15), 12363-12373CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
    Knowledge of the ibuprofen (IBP) adsorption isotherms is important to understand and to improve its depollution process. In this work, the double layer model with two energies was applied to simulate the adsorption isotherms of ibuprofen on raw activated and two chem. modified granular activated carbons, obtained exptl. at pH = 7 and at different temps. (298, 313 and 323 K). The chem. modified samples were obtained by treatment at 700°C under nitrogen flow and ultrasonic treatment in H2O2 soln. of the raw granulated activated carbon. The establishment of the model is based on a statistical physics approach, particularly on the grand canonical ensemble. The double layer model with two energies for each layer was found to be the best model to describe the adsorption process of ibuprofen. Using this model, the different adsorption isotherms of ibuprofen were described sterically and energetically through these parameters. The different parameters were interpreted as a function of temp. In addn. to this, the entropy, free enthalpy and the internal energy governing the adsorption process were calcd. and interpreted.
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  68. 68
    Zafar, M. N.; Amjad, M.; Tabassum, M.; Ahmad, I.; Zubair, M. SrFe2O4 Nanoferrites and SrFe2O4/Ground Eggshell Nanocomposites: Fast and Efficient Adsorbents for Dyes Removal. Journal of Cleaner Production 2018, 199, 983– 994,  DOI: 10.1016/j.jclepro.2018.07.204
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    68
    SrFe2O4 nanoferrites and SrFe2O4/ground eggshell nanocomposites: Fast and efficient adsorbents for dyes removal
    Zafar, Muhammad Nadeem; Amjad, Mufarah; Tabassum, Mehwish; Ahmad, Iqbal; Zubair, Muhammad
    Journal of Cleaner Production (2018), 199 (), 983-994CODEN: JCROE8; ISSN:0959-6526. (Elsevier Ltd.)
    In recent years nanomaterials are attracting much attention in water pollution treatment due to their greater surface area and unique properties. In this work, a micro emulsion method had been successfully utilized to synthesize novel strontium nanoferrites, SrFe2O4 an efficient adsorbent for both anionic dye erichrome black T and cationic dye methylene blue. To further improve the efficiency of SF, eggshells powder was employed as a support or co sorbent to produce another adsorbent named SF@EgP by combining EgP and SF using solvothermal method. The adsorbents were characterized by XRD, SEM techniques and further impendence spectroscopy and electrochem. characterization was also performed for SF. The SF and SF@EgP were tuned for EBT and MB removal and proved to be novel and efficient adsorbents and their adsorption efficiency was also compared with EgP. Using these model dyes, we investigated the influence of pH, adsorbent quantity, time and initial dyes concns. on adsorption. The adsorption process of EBT and MB was examd. by kinetics, isothermal and thermodn. modeling that resp. directed that the removal of dyes was much quicker. In addn., the SF and SF@EgP were regenerated and recycled successfully showing their reusability. In short these novel adsorbents not only tunable and showed reusability for cationic and anionic dyes with fast adsorption but also provide valuable clues towards synthesis and adsorption studies of other nanomaterials.
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    Yildirim, A.; Bulut, Y. Adsorption Behaviors of Malachite Green by Using Crosslinked Chitosan/Polyacrylic Acid/Bentonite Composites with Different Ratios. Environmental Technology & Innovation 2020, 17, 100560  DOI: 10.1016/j.eti.2019.100560
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    69
    Adsorption behaviors of malachite green by using crosslinked chitosan/polyacrylic acid/bentonite composites with different ratios
    Yildirim, Ayfer; Bulut, Yasemin
    Environmental Technology & Innovation (2020), 17 (), 100560CODEN: ETINBL; ISSN:2352-1864. (Elsevier B.V.)
    In this study, by using different quantities of methylenebisacrylamide (MBA) and acrylic acid (AA), chitosan/polyacrylic acid/bentonite composites (CCS/PAA/BNTs) were synthesized and used for the adsorption of malachite green (MG). The fourier transmission IR spectra, thermogravimetric anal.-DTA and SEM techniques were used to det. synthesized composites. The effects of initial concn., contact time, temp. and pH were investigated. Kinetic studies indicated that, due to the pseudo-second order model, correlation coeffs. (R2>0.98) were the best fit thus, by using kps, the activation energies (Ea) were calcd.(19.06, 15.64, 19.49, 8.29, 24.53 kJmol-1). The equil. data of MG agreed with the Langmuir model. The highest adsorption capacity calcd. was found as 384.62-454.55 mgg-1 for MG adsorption at 298-318 K. Thermodn. studies demonstrated that MG adsorption was endothermic, caused spontaneous reaction and increased the entropy between 298-318 K. The adsorption reactions of MG were revealed as physisorption (ΔH<80 kjmol-1). The optimum pH was found as 6. The CCS/PAA/BNT2 composite indicated the highest adsorption capacity and best thermal stability compared to the other composites.
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  70. 70
    Jiang, M.; Chen, L.; Niu, N. Enhanced Adsorption for Malachite Green by Functionalized Lignin Magnetic Composites: Optimization, Performance and Adsorption Mechanism. J. Mol. Struct. 2022, 1260, 132842  DOI: 10.1016/j.molstruc.2022.132842
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    70
    Enhanced adsorption for malachite green by functionalized lignin magnetic composites: Optimization, performance and adsorption mechanism
    Jiang, Minwen; Chen, Ligang; Niu, Na
    Journal of Molecular Structure (2022), 1260 (), 132842CODEN: JMOSB4; ISSN:0022-2860. (Elsevier B.V.)
    Herein, a novel kind of magnetic amino-modified lignin (MAL) sorbents was designed through a facile strategy based on Mannich reaction, which was used for removing a typical aquatic pollutant malachite green (MG). During the synthesis procedure, the 3-amino-propyltriethoxysilane was used as the cross-linker between aminated lignin and magnetic nanoparticles. The phys. and chem. structure of MAL were investigated through a series of characterization methods including FTIR, XRD, TGA, SEM, and XPS. The effect of pH shows that the adsorbent has excellent adsorption performance for MG at pH=7. According to the adsorption data, the adsorption process was in line with the Langmuir model and the pseudo-second-order model, indicating that the adsorption was monolayer adsorption and chemisorption. MAL showed excellent sorption capacity of 456.62 mg/g and high adsorption speed within 35 min. Thermodn. studies show that the adsorption is exothermic and spontaneous. Meanwhile, MAL shows good magnetic properties with the satn. magnetization intensities of 22.61 emu/g. In addn., the MAL could be easily recovered and reused at least five times, which performed good reusability. The mechanism of MG capture onto MAL can be mainly attributed to electrostatic attraction, hydrogen bonding, and π-π stacking. In a word, the as-prepd. MAL showed great potential for wastewater treatment due to its excellent adsorption efficiency, environmental friendliness, and superparamagnetic behavior.
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  71. 71
    Gupta, K.; Khatri, O. P. Reduced Graphene Oxide as an Effective Adsorbent for Removal of Malachite Green Dye: Plausible Adsorption Pathways. J. Colloid Interface Sci. 2017, 501, 11– 21,  DOI: 10.1016/j.jcis.2017.04.035
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    71
    Reduced graphene oxide as an effective adsorbent for removal of malachite green dye: Plausible adsorption pathways
    Gupta, Kanika; Khatri, Om P.
    Journal of Colloid and Interface Science (2017), 501 (), 11-21CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)
    Efficient removal of malachite green (MG) dye from simulated wastewater is demonstrated using high surface area reduced graphene oxide (rGO). The plausible interaction pathways between MG dye and rGO are deduced from nanostructural features (HRTEM) of rGO and spectroscopic analyses (FTIR and Raman). The high surface area (931 m2 gm-1) of rGO, π-π interaction between the arom. rings of MG dye and graphitic skeleton, and electrostatic interaction of cationic center of MG dye with π-electron clouds and neg. charged residual O functionalities of rGO collectively facilitate the adsorption of MG dye on the rGO. The rGO displays adsorption capacity ≤476.2 mg g-1 for MG dye. The thermodn. parameters calcd. from the temp. dependent isotherms suggested that the adsorption was a spontaneous and endothermic process. These results promise the potential of high surface area rGO for efficient removal of cationic dyes for wastewater treatment.
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    Sricharoen, P.; Kongsri, S.; Kukusamude, C.; Areerob, Y.; Nuengmatcha, P.; Chanthai, S.; Limchoowong, N. Ultrasound-Irradiated Synthesis of 3-Mercaptopropyl Trimethoxysilane-Modified Hydroxyapatite Derived from Fish-Scale Residues Followed by Ultrasound-Assisted Organic Dyes Removal. Sci. Rep. 2021, 11 (1), 5560,  DOI: 10.1038/s41598-021-85206-5
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    Ultrasound-irradiated synthesis of 3-mercaptopropyl trimethoxysilane-modified hydroxyapatite derived from fish-scale residues followed by ultrasound-assisted organic dyes removal
    Sricharoen, Phitchan; Kongsri, Supalak; Kukusamude, Chunyapuk; Areerob, Yonrapach; Nuengmatcha, Prawit; Chanthai, Saksit; Limchoowong, Nunticha
    Scientific Reports (2021), 11 (1), 5560CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)
    We report a novel method for the synthesis of 3-mercaptopropyl trimethoxysilane-modified hydroxyapatite (FHAP-SH) derived from fish-scale residues by using ultrasound irradn. SEM, transmission electron microscopy, energy-dispersive spectroscopy, X-ray diffraction, and Fourier transform IR spectroscopy were used for the FHAP-SH characterization. Then, the org. dye adsorption on the FHAP-SH was monitored through an ultrasound process. After the dye removal optimization, significant improvements were obsd. in the max. adsorption capacities for Congo Red (CR, 500 mg g-1), Coomassie Brilliant Blue G 250 (CB, 235 mg g-1), and Malachite Green (MG, 625 mg g-1). The adsorption behaviors of these dyes were fitted by using the Langmuir isotherm model with a high coeff. of detn. values ranging from 0.9985 to 0.9969. The adsorption of the three dyes onto FHAP-SH was an endothermic process based on the adsorption thermodn. model, while the adsorption kinetics anal. of the dyes presented a good alignment with the pseudo-second-order kinetics. The FHAP-SH exhibits a remarkably high adsorption capacity, is inexpensive, and fulfills the ecofriendly requirements of dye wastewater treatment, esp. in the textile industry.
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    Gao, M.; Wang, Z.; Yang, C.; Ning, J.; Zhou, Z.; Li, G. Novel Magnetic Graphene Oxide Decorated with Persimmon Tannins for Efficient Adsorption of Malachite Green from Aqueous Solutions. Colloids Surf., A 2019, 566, 48– 57,  DOI: 10.1016/j.colsurfa.2019.01.016
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    Novel magnetic graphene oxide decorated with persimmon tannins for efficient adsorption of malachite green from aqueous solutions
    Gao, Mingmin; Wang, Zhongmin; Yang, Chengxian; Ning, Jinliang; Zhou, Zhide; Li, Guiyin
    Colloids and Surfaces, A: Physicochemical and Engineering Aspects (2019), 566 (), 48-57CODEN: CPEAEH; ISSN:0927-7757. (Elsevier B.V.)
    Dyeing effluent is one of the main sources of textile wastewater, which has a seriously destructive impact on human health. A simple and effective way to remove dyes from the environment is required. In this paper, a new adsorbent, magnetic graphene oxide decorated with persimmon tannins (Fe3O4/PT/GO) composites, has been prepd. by one-step hydrothermal method for efficient adsorption of malachite green (MG) from aq. solns. The microstructure and compn. of the Fe3O4/PT/GO adsorbent were characterized by SEM, Fourier transform IR (FTIR) spectroscopy, Brunauer-Emmett-Teller (BET) anal., X-ray powder diffraction (XRD) and vibrating sample magnetometer (VSM). The Fe3O4/PT/GO adsorbent had excellent adsorption ability with the max. adsorption capacity of 560.58 mg/g at 308 K and pH 6.0. The adsorption capacity maintained 85.9% after five cycles. The adsorption process of MG conformed to the Langmuir isotherm model and pseudo-second order kinetic equations. In addn., the thermodn. studies indicated that the adsorption process is spontaneous and endothermic. All the exptl. results showed that the Fe3O4/PT/GO adsorbent had good adsorption capacity for removing MG from wastewater and can be quickly extd. from water under an external magnetic field.
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    Raval, N. P.; Shah, P. U.; Shah, N. K. Malachite Green “a Cationic Dye” and Its Removal from Aqueous Solution by Adsorption. Applied Water Science 2017, 7 (7), 3407– 3445,  DOI: 10.1007/s13201-016-0512-2
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    Malachite green "a cationic dye" and its removal from aqueous solution by adsorption
    Raval, Nirav P.; Shah, Prapti U.; Shah, Nisha K.
    Applied Water Science (2017), 7 (7), 3407-3445CODEN: AWSPCL; ISSN:2190-5495. (Springer GmbH)
    Adsorption can be efficiently employed for the removal of various toxic dyes from water and wastewater. In this article, the authors reviewed variety of adsorbents used by various researchers for the removal of malachite green (MG) dye from an aq. environment. The main motto of this review article was to assemble the scattered available information of adsorbents used for the removal of MG to enlighten their wide potential. In addn. to this, various optimal exptl. conditions (soln. pH, equil. contact time, amt. of adsorbent and temp.) as well as adsorption isotherms, kinetics and thermodn. data of different adsorbents towards MG were also analyzed and tabulated. Finally, it was concluded that the agricultural solid wastes and biosorbents such as biopolymers and biomass adsorbents have demonstrated outstanding adsorption capabilities for removal of MG dye.
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Cite this: ACS Omega 2023, 8, 51, 49347–49361
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Published December 12, 2023

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  • Abstract

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    Figure 1

    Figure 1. XRD patterns of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), and synthetic glauconite nanorods (GNRs) (D).

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    Figure 2

    Figure 2. SEM images of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), CTAB intercalated glauconite (D), and synthetic GNRs (E and F).

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    Figure 3

    Figure 3. HRTEM images of raw glauconite (A), in-depth scrolled glauconite with lattice fingers structures (B and C), and the synthetic GNRs after extensive sonication treatment (D–F).

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    Figure 4

    Figure 4. FTIR spectra of raw glauconite (A), DMSO intercalated glauconite (B), methoxy glauconite (C), and synthetic GNRs (D).

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    Figure 5

    Figure 5. EDX spectrum of the synthetic GNRs and the corresponding elemental composition.

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    Figure 6

    Figure 6. Plotted nitrogen adsorption/desorption isotherm curve of the synthetic GNR particles and the pore size distribution properties.

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    Figure 7

    Figure 7. Influence of the solution pH on the uptake of MG dye by GNRs.

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    Figure 8

    Figure 8. Influence of contact time on the uptake of MG by GNRs (A), intraparticle diffusion curve during the uptake of MG (B), fitting of the MG uptake data with the common kinetic models (C), influence of MG starting concentrations on the uptake capacities of GNRs (D), fitting of the MG uptake data with the classic Langmuir model (E), fitting of the MG uptake data with the classic Freundlich model (F), fitting of the MG uptake data with the classic D–R model (G), and fitting of the MG uptake data with the advanced monolayer equilibrium model of one site of energy (H).

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    Figure 9

    Figure 9. Variations in the quantity of MG molecules retained per site over the surface of GNRs (A), variations in the density of active sites with regard to temperature (B), fluctuations in the predicted uptake capacity of MG during the point of saturation of GNRs (C), shifts in entropy values in relation to MG concentration as well as temperature (D), variations in internal energy values with respect to MG concentration alongside temperature (E), and variations in enthalpy values as a function of MG concentration alongside temperature (F).

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    Figure 10

    Figure 10. Recyclability properties of the synthetic GNRs during the uptake of MG dye.

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      A natural piezoelec. quartz core was coated with environmentally friendly ZnO nanoparticles (GZn/PQz) for enhanced decontamination of ibuprofen (IBF) by adsorption and advanced oxidn. The adsorption properties were described based on the monolayer model of one energy site. The steric studies demonstrated a decline in active site d. (Nm) and the satn. adsorption capacities (Qsat) with increasing temp., and the best values were achieved at 25°C (Nm = 38.42 mg/g and Qsat = 145.6 mg/g). The no. of adsorbed IBF mols. (n) (>3 and <4) suggested the uptake of 3 or 4 IBF mols. per receptor site in a vertical orientation and by a multimol. mechanism. The adsorption energy values (-7.93 to -9.5 kJ/mol) suggest phys. uptake processes. The thermodn. functions reflected the exothermic and spontaneous properties of the reactions. GZn/PQz achieved IBF (50 mg/L) oxidn. percentages of 100%, 93.8%, and 100% after 80 min (photocatalyst), 360 min (piezoelec. catalyst), and 40 min (piezo-photocatalyst), resp. Hydroxyl radicals and superoxide radicals are essential oxidizing species during the oxidn. of IBF by GZn/PQz. Based on the detected intermediate compds., the oxidn. pathway of IBF by GZn/PQz involved hydroxylation, decarboxylation/demethylation, and ring-opening processes.
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      Abdel Salam, M.; Mokhtar, M.; Albukhari, S. M.; Baamer, D. F.; Palmisano, L.; Jaremko, M.; Abukhadra, M. R. Synthesis and Characterization of Green ZnO@polynaniline/Bentonite Tripartite Structure (G.Zn@PN/BE) as Adsorbent for As (V) Ions: Integration, Steric, and Energetic Properties. Polymers 2022, 14 (12), 2329,  DOI: 10.3390/polym14122329
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      Synthesis and Characterization of Green ZnO@polynaniline/Bentonite Tripartite Structure (G.Zn@PN/BE) as Adsorbent for As (V) Ions: Integration, Steric, and Energetic Properties
      Abdel Salam, Mohamed; Mokhtar, Mohamed; Albukhari, Soha M.; Baamer, Doaa F.; Palmisano, Leonardo; Jaremko, Mariusz; Abukhadra, Mostafa R.
      Polymers (Basel, Switzerland) (2022), 14 (12), 2329CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
      A green ZnO@polynaniline/bentonite composite (G.Zn@PN/BE) was synthesized as an enhanced adsorbent for As (V) ions. Its adsorption properties were assessed in comparison with the integrated components of bentonite (BE) and polyaniline/bentonite (PN/BE) composites. The G.Zn@PN/BE composite achieved an As (V) retention capacity (213 mg/g) higher than BE (72.7 mg/g) and PN/BE (119.8 mg/g). The enhanced capacity of G.Zn@PN/BE was studied using classic (Langmuir) and advanced equil. (monolayer model of one energy) models. Considering the steric properties, the structure of G.Zn@PN/BE demonstrated a higher d. of active sites (Nm = 109.8 (20°C), 108.9 (30°C), and 67.8 mg/g (40°C)) than BE and PN/BE. This declared the effect of the integration process in inducing the retention capacity by increasing the quantities of the active sites. The no. of adsorbed As (V) ions per site (1.76 up to 2.13) signifies the retention of two or three ions per site by a multi-ionic mechanism. The adsorption energies (from -3.07 to -3.26 kJ/mol) suggested phys. retention mechanisms (hydrogen bonding and dipole bonding forces). The adsorption energy, internal energy, and free enthalpy reflected the exothermic, feasible, and spontaneous nature of the retention process. The structure is of significant As (V) uptake capacity in the existence of competitive anions or metal ions.
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      AlHammadi, A. A.; Nasser, R.; Shaban, M. S.; Othman, S. I.; Khim, J. S.; Ajarem, J. S.; Allam, A. A.; Abukhadra, M. R. Insight into the Effect of Sulfonation Techniques on the Adsorption Properties of – SO3H Surface-Functionalized Coal as Adsorbent for Malachite Green Dye: Steric and Energetic Investigation. ACS Omega 2022, 7 (41), 36697– 36711,  DOI: 10.1021/acsomega.2c04985
      4
      Insight into the Effect of Sulfonation Techniques on the Adsorption Properties of -SO3H Surface-Functionalized Coal as Adsorbent for Malachite Green Dye: Steric and Energetic Investigation
      AlHammadi, Ali A.; Nasser, Rania; Shaban, Mohamed S.; Othman, Sarah I.; Khim, Jong Seong; Ajarem, Jamaan S.; Allam, Ahmed A.; Abukhadra, Mostafa R.
      ACS Omega (2022), 7 (41), 36697-36711CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      Natural coal (N.C) was sulfonated with sulfuric acid by normal stirring (MS.C) and sonication waves (SS.C) to obtain -SO3H functionalized coal as enhanced adsorbents of malachite green dye (MG). The sulfonated products exhibit enhanced surface area MS.C (27.2 m2/g) and SS.C (45.8 m2/g) as compared to N.C. SS.C achieved higher acid d. (14.2 mmol/g) and sulfur content (13.2 wt. %) as compared to MS.C. The impact of the sulfonation processes on the adsorption of MG was assessed based on the monolayer isotherm model of one energy. The MG Qsat of N.C (121.3 mg/g), MS.C (226.3 mg/g), and SS.C (296.4 mg/g) validate the significant effect of the sulfonation processes by the sonication waves. This is in agreement with the active site densities that reflect the satn. of SS.C by more active sites (180.74 mg/g) than MS.C (120.38 mg/g) and N.C (70.84 mg/g). The MS.C and SS.C can adsorb three MG mols. as compared to two mols. per site of N.C. The Gaussian energy (<8 kJ/mol) and adsorption energy (<40 kJ/mol) reflects the physisorption of MG involving van der Waals forces, hydrogen bonding, and dipole bonding forces. The thermodn. functions demonstrate the uptake of MG by exothermic, spontaneous, feasible reactions.
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      Benisha, R.; Amalanathan, M.; Aravind, M.; Mary, M. S. M.; Ahmad, A.; Tabassum, S.; Al-Qahtani, W. H.; Ahmad, I. Catharanthus Roseus Leaf Extract Mediated Ag-MgO Nanocatalyst for Photocatalytic Degradation of Congo Red Dye and Their Antibacterial Activity. J. Mol. Struct. 2022, 1262, 133005  DOI: 10.1016/j.molstruc.2022.133005
      5
      Catharanthus roseus leaf extract mediated Ag-MgO nanocatalyst for photocatalytic degradation of Congo red dye and their antibacterial activity
      Benisha, R.; Amalanathan, M.; Aravind, M.; Mary, M. Sony Michel; Ahmad, Awais; Tabassum, Sobia; Al-Qahtani, Wahidah H.; Ahmad, Ikram
      Journal of Molecular Structure (2022), 1262 (), 133005CODEN: JMOSB4; ISSN:0022-2860. (Elsevier B.V.)
      A simple and cost-effective green synthesis approach was used for the manuf. of MgO and Ag-MgO nanocomposites using Catharanthus roseus leaf ext. and its photocatalytic ability against congo red (CR) dye was investigated. UV-visible spectroscopy (UV-Vis), Fourier transform IR spectroscopy (FTIR), X-ray difraction (XRD), transmission electron microscope (TEM), energy-dispersive X-ray spectroscopy (EDX), and XPS were used to examine the synthesized MgO NPs and Ag-MgO nanocomposite. The XRD pattern of MgO nanoparticles and Ag-MgO nanocomposites reveals fcc structure. Spherical shaped NPs were confirmed using SEM and TEM anal. The EDX profile confirmed the presence of Mg, Ag, and O elements. The existence of functional group responsible for stabilizing Ag-MgO nanocomposite was verified using FTIR anal. According to XPS spectra, valencies and binding energies of MgO and Ag elements were found in the as-prepd. Ag-MgO nanocomposites. Ag-MgO NCs degraded congo red (CR) dye faster than pure MgO NPS under sunlight irradn. than pure MgO NPs. The effect of dopant concn. on lowering recombination between electrons and holes was linked to increased photocatalytic activity of Ag-MgO NCs. Antibacterial results show good antibacterial activity against gram-pos. (S. aureus) and gram-neg. (E-Coli) microbial pathogens. These findings revealed the environmental remediation potential of Ag-doped MgO NPs.
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      Taher, T.; Putra, R.; Rahayu Palapa, N.; Lesbani, A. Preparation of Magnetite-Nanoparticle-Decorated NiFe Layered Double Hydroxide and Its Adsorption Performance for Congo Red Dye Removal. Chem. Phys. Lett. 2021, 777, 138712  DOI: 10.1016/j.cplett.2021.138712
      6
      Preparation of magnetite-nanoparticle-decorated NiFe layered double hydroxide and its adsorption performance for congo red dye removal
      Taher, Tarmizi; Putra, Raden; Rahayu Palapa, Neza; Lesbani, Aldes
      Chemical Physics Letters (2021), 777 (), 138712CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
      Magnetite-nanoparticle-decorated NiFe LDH (MNPs@NiFe LDH) has been synthesized by the copptn. method followed by subsequent hydrothermal treatment. Material characterization was conducted using XRD, FTIR, SEM, BET surface area, and TG-DTA. MNPs@NiFe LDH exhibited high crystallinity, where the MNPs are uniformly distributed on its surface. MNPs@NiFe LDH showed higher adsorption capacity for congo red dye removal from an aq. soln. (79.6 mg/g). A further adsorption study, kinetics, isotherm, and thermodn. indicated that the adsorption mechanism is governed by ionic interaction between the pos. charged surface of the LDH and neg. charged dye mols.
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    7. 7
      Okasha, A. T.; Abdel-Khalek, A. A.; El-Sherbeeny, A. M.; Zoubi, W. A.; Abukhadra, M. R. Advanced Equilibrium Study on the Synthesis and Characterization of Mg-Doped Hydroxyapatite Nano-Fibers as a Potential Enhanced Adsorbent of Zn (II) and Malachite Green Dye. Materials Today Communications 2023, 35, 105883  DOI: 10.1016/j.mtcomm.2023.105883
      7
      Advanced equilibrium study on the synthesis and characterization of Mg-doped hydroxyapatite nano-fibers as a potential enhanced adsorbent of Zn (II) and malachite green dye
      Okasha, Alaa T.; Abdel-Khalek, Ahmed A.; El-Sherbeeny, Ahmed M.; Zoubi, Wail Al; Abukhadra, Mostafa R.
      Materials Today Communications (2023), 35 (), 105883CODEN: MTCAC7; ISSN:2352-4928. (Elsevier Ltd.)
      Novel Mg-doped hydroxyapatite nanofibers (Mg.HAPNFs) were synthesized using inexpensive natural phosphorite and a facile method. The as-synthesized Mg.HAPNFs were characterized using several anal. methods and used as excellent adsorbent for Zn2+ ions and malachite green (MG) dye. The exptl. adsorption capacities of the as-synthesized Mg.HAPNFs for Zn2+ ions and MG dye were 441.2 and 635.1 mg/g, resp., whereas the theor. adsorption capacities at satn. were 458.7 and 673.5 mg/g, resp. The kinetics of the Mg.HAPNFs adsorption reactions for Zn2+ ions and MG dye were described using the pseudo-first-order kinetic model. A homogeneous monolayer mechanism for the adsorption of Zn2+ ions and MG dye mols. onto Mg.HAPNFs was proposed by fitting the exptl. data with the theor. Langmuir isotherm. The advanced equil. study of the Mg.HAPNF-Zn2+ and Mg.HAPNF-MG adsorption systems demonstrated that each active site of Mg.HAPNF vertically adsorbed three Zn2+ ions (n = 2.04) and two MG dye mols. (n = 1.92) via multi-ionic processes. The effective d. of adsorption sites of Mg.HAPNFs for MG dye (547.78 mg/g) was higher than that for Zn2+ ions (224.56 mg/g). The Gaussian energies (4.20 kJ/mol (Zn2+ ions) and 5.37 kJ/mol (MG dye)), adsorption energies (-5.4 kJ/mol (Zn2+ ions) and - 17.85 kJ/mol (MG dye)), and exptl. data for the Mg.HAPNF adsorbent indicated that adsorption involved several phys. and chem. mechanisms (i.e., hydrogen bonding, dissoln.-pptn., van der Waals forces, ion exchange, and dipole-dipole interactions). Thermodn. studies revealed that Mg.HAPNFs spontaneously and exothermically adsorbed Zn2+ ions and MG dye mols.
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    8. 8
      Pathania, D.; Dhar, S.; Sharma, A.; Srivastava, A. K. Decolourization of Noxious Safranin-T from Waste Water Using Mangifera Indica as Precursor. Environmental Sustainability 2021, 4 (2), 355– 364,  DOI: 10.1007/s42398-020-00130-0
      8
      Decolourization of noxious safranin-T from waste water using Mangifera indica as precursor
      Pathania, Deepak; Dhar, Sunil; Sharma, Arush; Srivastava, A. K.
      Environmental Sustainability (2021), 4 (2), 355-364CODEN: ESNUAP; ISSN:2523-8922. (Springer)
      Abstr.: Bark prepd. from Mangifera indica has been employed for eradication of safranin-T. Structural anal. of bark was attempted using Fourier-transform IR spectroscopy (FTIR), thermogravimetric anal. (TGA), and SEM (SEM). The effect of several parameters was tested and optimized. The percentage adsorption of dye onto bark was found to increase with temp. and dictate endothermic adsorption. About 87% of dye removal was found at contact time of 80 min. The percentage of safranin-T dye removal increased with adsorbent dosage. Different isotherms like Langmuir, Freundlich, and Tempkin were studied to det. the adsorption mechanism. The adsorption capacity of bark was recorded to be 78.96 mg/g. Langmuir model rightly described the adsorption process with higher regression value (R2 = 0.99). The exptl. data was found close to using Langmuir isotherm. This confirms the monolayer adsorption of safranin-T dye onto bark. The kinetic study and intra-particle diffusion described that adsorption followed the pseudo-second-order kinetics with greater R2 value. The study confirmed the chem. adsorption of dye onto adsorbent. The different thermodn. processes confirmed the feasible, spontaneous and endothermic adsorption of dye using M. indica bark. Graphic abstr.: [graphic not available: see fulltext].
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    9. 9
      Abukhadra, M. R.; Mostafa, M.; El-Sherbeeny, A. M.; El-Meligy, M. A.; Nadeem, A. Instantaneous Adsorption of Synthetic Dyes from an Aqueous Environment Using Kaolinite Nanotubes: Equilibrium and Thermodynamic Studies. ACS Omega 2021, 6 (1), 845– 856,  DOI: 10.1021/acsomega.0c05430
      9
      Instantaneous adsorption of synthetic dyes from an aqueous environment using kaolinite nanotubes: Equilibrium and thermodynamic studies
      Abukhadra, Mostafa R.; Mostafa, Merna; El-Sherbeeny, Ahmed M.; El-Meligy, Mohammed A.; Nadeem, Ahmed
      ACS Omega (2021), 6 (1), 845-856CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      Innovative kaolinite nanotubes (KNTs) are synthesized utilizing a simple technique involving a sonication-induced exfoliation process, followed by chem. scrolling reactions. The KNTs as a material have high reactivity and promising surface area to be used in the purifn. of water from cationic dyes (safranin (SF) and malachite green (MG)) and anionic dyes (methyl orange (MO) and Congo red (CR)). The kinetic studies of the four dyes SF, MG, CR, and MO show an equilibration time interval of 240 min. The SF, MG, CR, and MO dyes' uptake reactions are in agreement with the kinetic behavior of the pseudo-first-order model and the equil. properties of the Langmuir model. Such modeling results, in addn. to the Gaussian energies from the Dubinin-Radushkevich (D-R) model (SF (1.01 kJ/mol), MG (1.08 kJ/mol), CR (1.11 kJ/mol), and MO (1.65 kJ/mol)), hypothesize monolayer adsorption of the four dyes by phys. reactions. The KNTs show theor. qmax values of 431.6, 489.9, 626.2, and 675.5 (mg/g) for SF, MG, CR, and MO, resp. The thermodn. examn. of SF, MG, CR, and MO adsorption reactions using KNTs verifies their adsorption by exothermic and spontaneous reactions. The KNT adsorbents achieve promising adsorption results in the presence of different coexisting ions and show significant recyclability properties. Therefore, the prodn. of KNTs from kaolinite shows a strong effect on inducing the textural, physicochem., and adsorption properties of clay layers as well as their affinity for different species of synthetic dyes.
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    10. 10
      Mohamed, F.; Abukhadra, M. R.; Shaban, M. Removal of Safranin Dye from Water Using Polypyrrole Nanofiber/Zn-Fe Layered Double Hydroxide Nanocomposite (Ppy NF/Zn-Fe LDH) of Enhanced Adsorption and Photocatalytic Properties. Science of The Total Environment 2018, 640–641, 352– 363,  DOI: 10.1016/j.scitotenv.2018.05.316
      10
      Removal of safranin dye from water using polypyrrole nanofiber/Zn-Fe layered double hydroxide nanocomposite (Ppy NF/Zn-Fe LDH) of enhanced adsorption and photocatalytic properties
      Mohamed, Fatma; Abukhadra, Mostafa R.; Shaban, Mohamed
      Science of the Total Environment (2018), 640-641 (), 352-363CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      Polypyrrole nanofiber/Zn-Fe layered double hydroxide (Ppy NF/Zn-Fe LDH) was synthesized as nanocomposite of enhanced adsorption and photocatalytic properties. The formation of the composite was confirmed by XRD, FT-IR, HSEM, HRTEM, BET surface area and UV-vis spectrophotometer. Ppy NF/Zn-Fe LDH composite exhibits clear enhancing in the sp. surface area and obvious reducing in the band gap energy (from 2.8 eV for Zn-Fe LDH to 2.31 eV for the composite). This was reflected in a considerable improvement in the adsorption capacity and photocatalytic removal of safranin dye. The adsorption capacity was enhanced by about 22% higher than Ppy NF and by 31% higher than Zn-Fe LDH. The photocatalytic removal was improved by 41.6% higher than Ppy NF and by about 54% higher than Zn-Fe LDH. The adsorption of safranin dye by the composite is chemisorption adsorption and occurs in a multilayer form. The complete photocatalytic removal of 5 mg/L of safranin dye can be achieved after 120 min illumination time using 0.05 g of the composite as photocatalyst and the best results can be obtained at neutral to alk. conditions. Realistic application of the composite for the removal of dye from raw water samples revealed the applicability of the product for the purifn. of tap water, groundwater, and sewage water. Moreover, it can be used for six cycles of safranin dye removal from water. The photocatalytic degrdn. process appears to be controlled by the created hydroxyl radicals and formed photogenerated holes as the dominant active oxidizing radicals.
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    11. 11
      Eltaweil, A. S.; Ali Mohamed, H.; Abd El-Monaem, E. M.; El-Subruiti, G. M. Mesoporous Magnetic Biochar Composite for Enhanced Adsorption of Malachite Green Dye: Characterization, Adsorption Kinetics. Thermodynamics and Isotherms. Advanced Powder Technology 2020, 31 (3), 1253– 1263,  DOI: 10.1016/j.apt.2020.01.005
      There is no corresponding record for this reference.
    12. 12
      Rabie, A. M.; Abukhadra, M. R.; Rady, A. M.; Ahmed, S. A.; Labena, A.; Mohamed, H. S. H.; Betiha, M. A.; Shim, J.-J. Instantaneous Photocatalytic Degradation of Malachite Green Dye under Visible Light Using Novel Green Co–ZnO/Algae Composites. Res. Chem. Intermed. 2020, 46 (3), 1955– 1973,  DOI: 10.1007/s11164-019-04074-x
      12
      Photocatalytic degradation of malachite green under visible light using green Co-ZnO/algae composites
      Rabie, Abdelrahman M.; Abukhadra, Mostafa R.; Rady, Ahmed M.; Ahmed, Sayed A.; Labena, Ahmed; Mohamed, Hussein S. H.; Betiha, Mohamed A.; Shim, Jae-Jin
      Research on Chemical Intermediates (2020), 46 (3), 1955-1973CODEN: RCINEE; ISSN:0922-6168. (Springer)
      Abstr.: Nano-ZnO and Co-ZnO supported algae (Sargassum species) were synthesized as a novel composite of promising photocatalytic activities in decolorization of malachite green dye under a visible light source. The composites were characterized by different anal. techniques, and the results confirmed the loading process and the formation of composites of low band gap energies for ZnO/algae composite (2.45 eV) and Co-ZnO/algae composite (2.32 eV). The composites were used as photocatalysts for the rapid degrdn. of malachite green dye (MG) within the visible light zone. The synthetic catalysts showed stunning photocatalytic activities reflected in the complete degrdn. of 5 mg/L of MG after 10 min using 0.06 g of ZnO/algae and 0.05 g of Co-ZnO/algae at pH 7. Also, the studied composites showed high efficiency in the degrdn. of higher MG concn. (10 mg/L and 15 mg/L). The photocatalytic performances were enhanced by 58% for ZnO/algae and about 75% for Co-ZnO/algae as compared to pure ZnO without support. Moreover, they have high reusability properties and are applied effectively in seven cycles of MG degrdn. reusing tests. The active species trapping tests reflected the dominance of the electron-hole pairs in the visible light degrdn. of MG by ZnO/algae. For Co-ZnO/algae composite, the degrdn. mechanism appears to be controlled by both the electron-hole pairs and hydroxyl radicals with a similar effect.
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    13. 13
      Saad, A. M.; Abukhadra, M. R.; Abdel-Kader Ahmed, S.; Elzanaty, A. M.; Mady, A. H.; Betiha, M. A.; Shim, J.-J.; Rabie, A. M. Photocatalytic Degradation of Malachite Green Dye Using Chitosan Supported ZnO and Ce–ZnO Nano-Flowers under Visible Light. Journal of Environmental Management 2020, 258, 110043  DOI: 10.1016/j.jenvman.2019.110043
      13
      Photocatalytic degradation of malachite green dye using chitosan supported ZnO and Ce-ZnO nano-flowers under visible light
      Saad, Alaa Magdy; Abukhadra, Mostafa R.; Abdel-Kader Ahmed, Sayed; Elzanaty, Ali M.; Mady, Amr H.; Betiha, Mohamed A.; Shim, Jae-Jin; Rabie, Abdelrahman M.
      Journal of Environmental Management (2020), 258 (), 110043CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
      Two types of chitosan-based composites (chitosan/ZnO and chitosan/Ce-ZnO composites) were synthesized under microwave irradn. and characterized as advanced catalysts of enhanced photocatalytic activity under the visible light. The morphol. investigation reflected the formation of ZnO and Ce doped ZnO at stunning micro flowers of nano limps. Addnl., the optical studies reflected a redn. in the bandgap of ZnO from 3.3 eV to 2.85 eV and 2.5 eV after supporting it onto chitosan chains and after doping it with cerium, resp. The synthetic composites were applied in photocatalytic removal of malachite green dye under a visible light source. The synthetic CH/ZnO and CH/Ce-ZnO showed enhancement in the photocatalytic removal of M. G by 54% and 87%, resp., as compared to the pure ZnO. The synthetic composites are of high stability and can be reused for five photocatalytic degrdn. cycles at stunning removal percentages. The main oxidizing radicals during the removal of M. G by CH/ZnO are the generated electron-hole pairs as well as the hydroxyl radicals. The effective species in CH/Ce-ZnO photocatalytic system are the photogenerated hydroxyl radicals followed by the electron-hole pairs.
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    14. 14
      Ofudje, E. A.; Adedapo, A. E.; Oladeji, O. B.; Sodiya, E. F.; Ibadin, F. H.; Zhang, D. Nano-Rod Hydroxyapatite for the Uptake of Nickel Ions: Effect of Sintering Behaviour on Adsorption Parameters. Journal of Environmental Chemical Engineering 2021, 9 (5), 105931  DOI: 10.1016/j.jece.2021.105931
      14
      Nano-rod hydroxyapatite for the uptake of nickel ions: Effect of sintering behaviour on adsorption parameters
      Ofudje, Edwin Andrew; Adedapo, Adebusayo Emmanuel; Oladeji, Olugbenga Bowale; Sodiya, Ezekiel Folorunso; Ibadin, Francis Hope; Zhang, Dan
      Journal of Environmental Chemical Engineering (2021), 9 (5), 105931CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
      Sorption studies in batch approach were carried out to investigate the elimination of Ni(II) ions from aq. soln. by fish scale derived nano-rod hydroxyapatite (FSDNHA) obtained via thermal decompn. at 800 and 900 oC resp. The effects of Ni2+ concn., contact time, pH, FSDNHA dose and temp. on elimination process were examd. Adsorption studies showed that max. uptake amt. of Ni2+ was attained at initial Ni2+concn. of 240 mg L-1, sorption time of 120 min, FSDNHA dose of 40 mg and soln. pH of 6.0. The highest value of R2 obtained for Langmuir, Temkin, and Freundlich isotherms models are (0.996, 0.994, and 0.990) for FSDNHA-800 and (0.998, 0.986, and 0.992) for FSDNHA-900 resp. The values of the max. monolayer adsorption capacities obtained from Langmuir isotherm for FSDNHA-800 and FSDNHA-900 are 114.151 and 183.321 mg g-1 resp. Kinetic modeling of the adsorption data clearly revealed that the sorption of Ni2+ onto the active sites of the FSDNHA surface was governed by Pseudo-first-order kinetic model. Thermodn. parameters of Gibbs free energy (ΔG°), enthalpy (ΔH°) and entropy change (ΔS°) revealed that the sorption of Ni2+on FSDNHA was spontaneous, feasible and exothermic in nature. Well resolved peaks of a characteristic pure hydroxyapatite (HA) contg. hydroxyl, phosphate and carbonate groups were obtained as the major functional groups responsible for the uptake of Ni2+, while the morphol. anal. by FE-SEM and TEM revealed a nano-rod shape. This current study showed that Ni2+ removal by FSDNHA compared favorable with other adsorbents and is feasible.
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    15. 15
      Shahid, M.; Farooqi, Z. H.; Begum, R.; Arif, M.; Irfan, A.; Azam, M. Extraction of Cobalt Ions from Aqueous Solution by Microgels for In-Situ Fabrication of Cobalt Nanoparticles to Degrade Toxic Dyes: A Two Fold-Environmental Application. Chem. Phys. Lett. 2020, 754, 137645  DOI: 10.1016/j.cplett.2020.137645
      15
      Extraction of cobalt ions from aqueous solution by microgels for in-situ fabrication of cobalt nanoparticles to degrade toxic dyes: Two fold-environmental application
      Shahid, Muhammad; Farooqi, Zahoor H.; Begum, Robina; Arif, Muhammad; Irfan, Ahmad; Azam, Muhammad
      Chemical Physics Letters (2020), 754 (), 137645CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
      Microgels were obtained by method of free radical pptn. polymn. and characterized by TEM, DLS and FTIR. Adsorption of Co2+ ions was studied under various conditions of pH, concn. of metal ions and that of microgels. Different adsorption isotherms were applied to study mechanism of adsorption process. Kinetics and mechanism of the adsorption process was investigated by pseudo 1st order, pseudo 2nd order and intra-particle diffusion modeling. In situ redn. of Co2+ ions loaded into the polymer microgel was carried out to get hybrid system for catalytic degrdn. of 4-nitrophenol, Eosin and Methylene blue.
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    16. 16
      Sayed, I. R.; Farhan, A. M.; AlHammadi, A. A.; El-Sayed, M. I.; Abd El-Gaied, I. M.; El-Sherbeeny, A. M.; Al Zoubi, W.; Ko, Y. G.; Abukhadra, M. R. Synthesis of Novel Nanoporous Zinc Phosphate/Hydroxyapatite Nano-Rods (ZPh/HPANRs) Core/Shell for Enhanced Adsorption of Ni2+ and Co2+ Ions: Characterization and Application. J. Mol. Liq. 2022, 360, 119527  DOI: 10.1016/j.molliq.2022.119527
      16
      Synthesis of novel nanoporous zinc phosphate/hydroxyapatite nano-rods (ZPh/HPANRs) core/shell for enhanced adsorption of Ni2+ and Co2+ ions: Characterization and application
      Sayed, Islam R.; Farhan, Amna M.; AlHammadi, Ali A.; El-Sayed, Mohamed I.; Abd El-Gaied, Ibrahim M.; El-Sherbeeny, Ahmed M.; Al Zoubi, Wail; Ko, Young Gun; Abukhadra, Mostafa R.
      Journal of Molecular Liquids (2022), 360 (), 119527CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
      Novel nanoporous zinc phosphate/hydroxyapatite nano-rods core/shell (ZPh/HPANRs) was synthesized and characterized as a modified form of hydroxyapatite with superior Ni2+ and Co2+ adsorption capacities. The ZPh/HPANRs structure exhibits satn. adsorption capacities of 515.4 mg/g (Ni2+) and 758 mg/g (Co2+). The Ni2+ and Co2+ uptake reactions by ZPh/HPANRs follow the theor. behavior of Pseudo-First order and Pseudo-Second order kinetics, resp. The assumptions of the classic Langmuir isotherm and advanced Monolayer model with one energy site were applied to illustrate the equil. properties of both Ni2+ and Co2+ uptake reactions. Considering the steric parameters, the nos. of adsorbed Ni2+ (n = 1.52-2.58) and Co2+ (n = 1.07-2.55) suggest their adsorption as two or three metal ions per each active site of ZPh/HPANRs by multi-ionic processes and in a vertical orientation. The structure show higher active site d. for the Co2+ (Nm = 702.6 mg/g) than Ni2+ ions (Nm = 339.14 mg/g). The Gaussian energies (Ni2+ (3.13-4.49 kJ/mol) and Co2+ (8.63-9.44 kJ/mol)), adsorption energies (Ni2+ (-27.3 to -28.49 kJ/mol) and Co2+ (-25.11 to -28.2 kJ/mol)), FT-IR anal. and EDX anal. demonstrate complex chem. (pptn. and chem. complexation), phys. (hydrogen bonding), and ion exchange mechanisms. The thermodn. functions display the spontaneous and exothermic properties of the Ni2+ and Co2+ uptake reactions.
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    17. 17
      Albukhari, S. M.; Salam, M. A.; Abukhadra, M. R. Effective Retention of Inorganic Selenium Ions (Se (VI) and Se (IV)) Using Novel Sodalite Structures from Muscovite; Characterization and Mechanism. Journal of the Taiwan Institute of Chemical Engineers 2021, 120, 116– 126,  DOI: 10.1016/j.jtice.2021.02.026
      17
      Effective retention of inorganic Selenium ions (Se (VI) and Se (IV)) using novel sodalite structures from muscovite; characterization and mechanism
      Albukhari, Soha M.; Salam, Mohamed Abdel; Abukhadra, Mostafa R.
      Journal of the Taiwan Institute of Chemical Engineers (2021), 120 (), 116-126CODEN: JTICA8; ISSN:1876-1070. (Elsevier B.V.)
      Muscovite flakes were applied in the synthesis of three types of sodalite with different morphologies by hydrothermal processes for 24 h, 48 h, and 72 h. The synthetic sample after 72 h (S-72) showed the best surface area (105 m2/g), morphol. features, and ion exchange capacity (71.3 meq/100 g). The S-72 was applied for effective retention of both Se (VI) and Se (IV) ions in batch adsorption studies. The retention capacities of Se (VI) and Se (IV) ions using S-72 sodalite are 149 mg/g and 255 mg/g, resp. after an equilibration time of 300 min and 360 min. The kinetic assessment suggested Pseudo-second order behavior for the retention of both Se (VI) and Se (IV). The equil. studies of their retention reactions demonstrated Langmuir isotherm behavior and monolayer form for the homogeneously adsorbed Se (VI) and Se (IV) ions on the surface of sodalite. The Gaussian energies (> 8 KJ/mol), enthalpies (< 80 KJ/mol), and Gibbs free energies (< 40 KJ/mol) for both Se (VI) and Se (IV) suggested phys. reactions related to coulumbic attractive forces or ion exchange process. Based on the thermodn. investigations, the Se (VI) and Se (IV) retention reactions are of exothermic, favorable, and spontaneous properties. The removal percentages of Se (VI) and Se (IV) ions by sodalite in the coexisting of Pb2+, Zn2+, PO-34, and NH4+ ions are of significant values either in pH 2 or pH 7.
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    18. 18
      Raju, CH. A. I.; Anitha, J.; Mahalakshmi Kalyani, R.; Satyanandam, K.; Jagadeesh, P. Sorption of Cobalt Using Marine Macro Seaweed Graciliariacorticatared Algae Powder. Materials Today: Proceedings 2021, 44, 1816– 1827,  DOI: 10.1016/j.matpr.2020.12.009
      18
      Sorption of cobalt using marine macro seaweed graciliariacorticatared algae powder
      Raju, CH. A. I.; Anitha, J.; Mahalakshmi Kalyani, R.; Satyanandam, K.; Jagadeesh, P.
      Materials Today: Proceedings (2021), 44 (7_Part_1), 1816-1827CODEN: MTPAC4; ISSN:2214-7853. (Elsevier Ltd.)
      Heavy metals are perilous contaminations that may exist in marine, ground, modern and even treated waste waters. Defilement of watery situations by weighty metals is an overall ecol. issue because of their poisonous impacts and their collection through the natural pecking order. Because of fast advancement of mech. exercises lately, the degrees of weighty metals in water frameworks, which have considerably expanded after some time, will prompt unnecessary arrival of the hefty metals into nature. Thus, it's important to eliminate these metals from mech. effluents before releasing watery squanders into condition. The present experimentation is aimed at removal of cobalt using gracilariacorticata red algae powder. The parameters varied are contact time, pH, sorbent size, dosage of sorbent, initial concn. and temp. The kinetics studied arelagergren first order and pseudo second order. Isotherms varied are Langmuir, Freundlich and Temkin. Optimization was carried out using Artificial neural networks and response surface methodol. The results were compared and are in good agreement.
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    19. 19
      Zhang, Y.; Hui, C.; Wei, R.; Jiang, Y.; Xu, L.; Zhao, Y.; Du, L.; Jiang, H. Study on Anionic and Cationic Dye Adsorption Behavior and Mechanism of Biofilm Produced by Bacillus Amyloliquefaciens DT. Appl. Surf. Sci. 2022, 573, 151627  DOI: 10.1016/j.apsusc.2021.151627
      19
      Study on anionic and cationic dye adsorption behavior and mechanism of biofilm produced by Bacillus amyloliquefaciens DT
      Zhang, Yiping; Hui, Cai; Wei, Ran; Jiang, Ying; Xu, Ligen; Zhao, Yuhua; Du, Linna; Jiang, Hui
      Applied Surface Science (2022), 573 (), 151627CODEN: ASUSEE; ISSN:0169-4332. (Elsevier B.V.)
      Biofilm produced by Bacillus amyloliquefaciens DT was reported to be able to remove crystal violet from water. However, there is no report on the ability of biofilm to remove other dyes. Here, we used methyl blue (MB; anionic) and malachite green (MG; cationic) as model dyes and investigated the behaviors and mechanisms of their adsorption by bacterial biofilm. Biofilm surface morphol., functional groups, and chem. constituents were characterized. XPS and Fourier transform IR spectroscopy results demonstrated that the relevant adsorptive functional groups were C-N bond/-NH3-and C-N bond/O=P(C)-O- for MB and MG adsorption, resp. Isothermic and kinetic models revealed that biofilm adsorbs MB heterogeneously via chemisorption and intraparticle diffusion. In contrast, biofilm adsorbs MG mainly by phys. interaction. Biofilm adsorption capacities were substantially higher than those for most other adsorbents. Hence, biofilm is promising as an anionic and cationic dye adsorbent for wastewater treatment.
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    20. 20
      Çiftçi, H. Removal of Methylene Blue from Water by Ultrasound-Assisted Adsorption Using Low-Cost Bentonites. Chem. Phys. Lett. 2022, 802, 139758  DOI: 10.1016/j.cplett.2022.139758
      20
      Removal of methylene blue from water by ultrasound-assisted adsorption using low-cost bentonites
      Ciftci, Hakan
      Chemical Physics Letters (2022), 802 (), 139758CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
      This study focused on the comparison of ultrasound-assisted (UA) and conventional (shaking or stirring) adsorption techniques, taking into account the time-dependent adsorption capacities. Six different bentonite samples were used as adsorbents, and methylene blue (MB) was used as adsorbate. Effects of pH, contact time, MB initial concn., and temp. on the UA-adsorption were also investigated. XRD analyzes showed that all the bentonite samples were mostly composed of montmorillonite clay minerals, while XRF analyzes showed that the samples contained high percentage of silicon and aluminum oxides (≥70 wt%). Maximum zeta potential values (37.1-42.1 mV) were measured at pH 12 and, to confirm this, max. adsorption capacities were also detd. at this point. Ultrasound irradn. significantly increased the adsorption capacities of all bentonite samples in the early stages. For example, the adsorption capacity of the B-1 bentonite sample was measured as 388 mg/g by UA-adsorption at the first 5th minute, while it was 286 mg/g by conventional (C) adsorption technique at the same time. All bentonite samples showed increasing adsorption capacity with increased temp. confirming endothermic reaction. Maximum adsorption capacities of B-1, B-2, B-3, B-4, B-5, and B-6 bentonite samples with the 96-100% MB removal percentages at selected conditions (pH: 11-12, temp.: 25°C, contact time: 60 min, and MB initial concns. for B-1: 800, B-2: 700, B-3,4: 650, B-5: 600, and B-6: 500 mg/L) were measured as 398, 342, 320, 296, 288, and 243 mg/g, resp. Pseudo-second-order kinetic model and Langmuir isotherm model with higher correlation coeffs. were found to be more suitable to explain the adsorption of MB cations onto bentonites. In addn., max. adsorption capacities of B-1, B-2, B-3, B-4, B-5, and B-6 samples at 25°C calcd. from Langmuir isotherm data detd. as 500, 454.5, 400, 384.6, 370, and 357.1 mg/g, resp.
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    21. 21
      Alqahtani, M. D.; Nasser, N.; AlZahrani, S. A.; Allam, A. A.; Abukhadra, M. R. Characterization of Kaolinite Single Methoxy Nano-Sheets as Potential Carriers of Oxaliplatin Drug of Enhanced Loading, Release, and Cytotoxicity Properties During the Treatment of Colorectal Cancer. Journal of Inorganic and Organometallic Polymers and Materials 2023, 33 (7), 2111– 2126,  DOI: 10.1007/s10904-023-02634-8
      21
      Characterization of Kaolinite Single Methoxy Nano-Sheets as Potential Carriers of Oxaliplatin Drug of Enhanced Loading, Release, and Cytotoxicity Properties During the Treatment of Colorectal Cancer
      Alqahtani, Mashael D.; Nasser, Nourhan; AlZahrani, Saleha A.; Allam, Ahmed A.; Abukhadra, Mostafa R.
      Journal of Inorganic and Organometallic Polymers and Materials (2023), 33 (7), 2111-2126CODEN: JIOPAY; ISSN:1574-1443. (Springer International Publishing AG)
      Kaolinite mineral was exfoliated into single nano-sheets (EXFK) and functionalized by methanol forming novel methoxy kaolinite nanosheet (MX/EXFK) as effective carrier of oxaliplatin drug (OXP). The functionalization of EXFK notably enhanced the loading properties to 433 mg/g (MX/EXFK) instead of 304.9 mg/g (EXFK). The loading reactions by EXFK and MX/EXFK follow the Pseudo-first order kinetics (R2 > 0.94) and classic Langmuir isotherm (R2 = 0.99). MX/EXFK shows enhanced active sites d. (109.9 mg/g) as compared to 66.3 mg/g (EXFK) and each site can be loaded with 4 mols. by multi-mol. mechanism. The encapsulation energy (< 40 kJ/mol) and Gaussian energy (< 8 kJ/mol) validates the dominant phys. encapsulation mechanism of OXP. The release behavior of OXP from MX/EXFK demonstrates continuous and controlled profiles up to 100 h (pH) and 180 h (phosphate buffer). The release processes exhibit non-Fickian transport properties according to the kinetic studies and diffusion exponent values (0.52-0.61). The synthetic structures exhibit considerable cytotoxicity effect on HCT-116 cancer cell lines EXFK (71.4% cell viability); MX/EXFK (12.08% cell viability). Moreover, these carriers induce the cytotoxic effects of OXP significantly OXP/EXFK (2.04% cell viability); OXP/MX/EXFK (0.95% cell viability).
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    22. 22
      Almahri, A. The Solid-State Synthetic Performance of Bentonite Stacked Manganese Ferrite Nanoparticles: Adsorption and Photo-Fenton Degradation of MB Dye and Antibacterial Applications. Journal of Materials Research and Technology 2022, 17, 2935– 2949,  DOI: 10.1016/j.jmrt.2022.02.052
      22
      The solid-state synthetic performance of bentonite stacked manganese ferrite nanoparticles: adsorption and photo-fenton degradation of MB dye and antibacterial applications
      Almahri, Albandary
      Journal of Materials Research and Technology (2022), 17 (), 2935-2949CODEN: JMRTAL; ISSN:2238-7854. (Elsevier B.V.)
      The development of nanocomposites for environmental demands is a challenge due to numerous precautions, including tailoring recyclable agents. In this work, bentonite clay (B. Clay)/manganese ferrite (MnFe2O4) nanocomposites have been fabricated via a solid-state technique that is green, efficient, and scalable. The obtained composites have been characterized using FTIR, SEM, and TEM. From the results, MnFe2O4 was configured in spherical shape during the interaction with B. Clay, reflecting the quality of applications. The studied av. max. height of the roughness (Rtm) changes from 151.7 to 107.3 and increases to 141.5 for pure B. Clay, MnFe2O4, and the nanocomposite, resp. The surface area for the nanocomposite was around 85.45 m2/g compared with 57. 46 m2/g for MnFe2O4. The magnetic domain has been enhanced exponentially to be 19.93 emu/g after solid synthesis of MnFe2O4 with B. Clay. The adsorption property was more significant in the case of MnFe2O4/B. clay to reach 71.6% decolorization of methylene blue (MB). Otherwise, under light illumination, the phytoremediation Fe3+ is reduced to Fe2+, accelerating switching on/off Fe3+/Fe2+ cycle stability to exhibit strong hydroxyl radicals able to destroy MB within 8 min. Also, at 100μg/mL concn., the prepd. MnFe2O4/B. Clay was aggressive against Staphylococcus aureus, Bacillus subtilis, Pseudomonas aeruginosa, and Escherichia coli.
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    23. 23
      Dardir, F. M.; Mohamed, A. S.; Abukhadra, M. R.; Ahmed, E. A.; Soliman, M. F. Cosmetic and Pharmaceutical Qualifications of Egyptian Bentonite and Its Suitability as Drug Carrier for Praziquantel Drug. European Journal of Pharmaceutical Sciences 2018, 115, 320– 329,  DOI: 10.1016/j.ejps.2018.01.041
      23
      Cosmetic and pharmaceutical qualifications of Egyptian bentonite and its suitability as drug carrier for Praziquantel drug
      Dardir, Fatma M.; Mohamed, Aya S.; Abukhadra, Mostafa R.; Ahmed, Ezzat A.; Soliman, Mamdouh F.
      European Journal of Pharmaceutical Sciences (2018), 115 (), 320-329CODEN: EPSCED; ISSN:0928-0987. (Elsevier B.V.)
      The aim of this paper is to characterize and evaluate newly discovered bentonite deposits in Egypt for pharmaceutical and cosmetic applications as well as its suitability as carrier for Praziquantel drug. The study was performed for the raw bentonite sample, purified bentonite sample and alkali activated purified bentonite sample. The raw bentonite sample composed mainly of montmorillonite contaminated by little amts. of quartz and calcite, while the purified sample composed of montmorillonite without detected mineral impurities and matches the mineralogical properties of Wyoming bentonite as an international std. Geochem., the studied raw and purified samples appear to high purity with a chem. compn. close to those of Wyoming bentonite and match the pharmacopeia specifications. The chem. properties in addn. to the textural properties of the surface area, porosity, particle size distribution qualify the bentonite products to use as a function in powder, emulsion and creams. Investigation of pharmacopeia properties of pH, sedimentation vol. and swelling capacity revealed the suitability of the raw and purified samples for pharmaceutical and cosmetic applications. Moreover, the microbiol. tests indicated that the samples free from harmful microbial pathogens. At the optimum conditions of time (240 min), bentonite dose (250 mg) and reaction temp. (60°C), the obtained encapsulation percentages of Praziquantel drug are 62%, 78.4% and 93.2% for raw bentonite, purified and alkali activated bentonite, resp. The releasing percentage of the drug using an intestinal buffer at pH 7.4 is more efficient and the max. obtained values were obtained after 420 min. The obtained releasing values are 71%, 79.2% and 87.4% for raw bentonite, purified bentonite and alkali activated bentonite, resp.
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    24. 24
      Alqahtani, M. D.; Nasser, N.; Bin Jumah, M. N.; AlZahrani, S. A.; Allam, A. A.; Abukhadra, M. R.; Bellucci, S. Insight into the Morphological Properties of Nano-Kaolinite (Nanoscrolls and Nanosheets) on Its Qualification as Delivery Structure of Oxaliplatin: Loading, Release, and Kinetic Studies. Molecules 2023, 28 (13), 5158,  DOI: 10.3390/molecules28135158
      24
      Insight into the Morphological Properties of Nano-Kaolinite (Nanoscrolls and Nanosheets) on Its Qualification as Delivery Structure of Oxaliplatin: Loading, Release, and Kinetic Studies
      Alqahtani, Mashael Daghash; Nasser, Nourhan; Bin Jumah, May N.; AlZahrani, Saleha A.; Allam, Ahmed A.; Abukhadra, Mostafa R.; Bellucci, Stefano
      Molecules (2023), 28 (13), 5158CODEN: MOLEFW; ISSN:1420-3049. (MDPI AG)
      Natural kaolinite underwent advanced morphol.-modification processes that involved exfoliation of its layers into sepd. single nanosheets (KNs) and scrolled nanoparticles as nanotubes (KNTs). Synthetic nanostructures have been characterized as advanced and effective oxaliplatin-medication (OXAP) delivery systems. The morphol.-transformation processes resulted in a remarkable enhancement in the loading capacity to 304.9 mg/g (KNs) and 473 mg/g (KNTs) instead of 29.6 mg/g for raw kaolinite. The loading reactions that occurred by KNs and KNTs displayed classic pseudo-first-order kinetics (R2 > 0.90) and conventional Langmuir isotherms (R2 = 0.99). KNTs exhibit a higher active site d. (80.8 mg/g) in comparison to KNs (66.3 mg/g) and raw kaolinite (6.5 mg/g). Furthermore, compared to KNs and raw kaolinite, each site on the surface of KNTs may hold up to six mols. of OXAP (n = 5.8), in comparison with five mols. for KNs. This was accomplished by multi-mol. processes, including phys. mechanisms considering both the Gaussian energy (<8 KJ/mol) and the loading energy (<40 KJ/mol). The release activity of OXAP from KNs and KNTs exhibits continuous and regulated profiles up to 100 h, either by KNs or KNTs, with substantially faster characteristics for KNTs. Based on the release kinetic investigations, the release processes have non-Fickian transport-release features, indicating cooperative-diffusion and erosion-release mechanisms. The synthesized structures have a significant cytotoxicity impact on HCT-116 cancer cell lines (KNs (71.4% cell viability and 143.6 g/mL IC-50)); KNTs (11.3% cell viability and 114.3 g/mL IC-50). Addnl., these carriers dramatically increase OXAPs cytotoxicity (2.04% cell viability, 15.4 g/mL IC-50 (OXAP/KNs); 0.6% cell viability, 4.5 g/mL IC-50 (OXAP/KNTs)).
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    25. 25
      Singh, R.; Dutta, S. The Role of pH and Nitrate Concentration in the Wet Chemical Growth of Nano-Rods Shaped ZnO Photocatalyst. Nano-Structures & Nano-Objects 2019, 18, 100250,  DOI: 10.1016/j.nanoso.2019.01.009
      25
      The role of pH and nitrate concentration in the wet chemical growth of nano-rods shaped ZnO photocatalyst
      Singh, Rohini; Dutta, Suman
      Nano-Structures & Nano-Objects (2019), 18 (), 100250CODEN: NNAAH5; ISSN:2352-507X. (Elsevier B.V.)
      ZnO nano-rods were synthesized via wet chem. method at different nitrate concn. and pH value. The effect of pH and nitrate concn. on the size and morphol. of the prepd. ZnO photocatalysts have been investigated by particle size distribution anal. and Field emission SEM resp. Addnl., UV-Visible spectroscopy and energy dispersive studies and were carried out to confirm the optical and compositional properties of the prepd. ZnO powder. The estd. band gap of the as prepd. ZnO photocatalysts at different pH and nitrate concn. calcd. on the basis of Kubelka-Munk function was found to be in the range of ∼ 2.7-3.6 eV. Field emission scanning (FE-SEM) and transmission electron microscopic (TEM) observations reveal rod-like morphol. The photocatalytic activity of prepd. ZnO photocatalysts was evaluated by photo degrdn. of the mixt. of Methylene Blue (MB) and Rhodamine 6G (Rh 6G) soln. under simulated solar radiation. Vol. of hydrogen evolution was recorded in the presence of prepd. ZnO photocatalysts in 2 h. Nitrate concn., and pH value showed a significant effect on the optical and morphol. behavior of the prepd. ZnO powd. photocatalysts.
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    26. 26
      Tan, D.; Yuan, P.; Dong, F.; He, H.; Sun, S.; Liu, Z. Selective Loading of 5-Fluorouracil in the Interlayer Space of Methoxy-Modified Kaolinite for Controlled Release. Appl. Clay Sci. 2018, 159, 102– 106,  DOI: 10.1016/j.clay.2017.04.008
      26
      Selective loading of 5-fluorouracil in the interlayer space of methoxy-modified kaolinite for controlled release
      Tan, Daoyong; Yuan, Peng; Dong, Faqin; He, Hongping; Sun, Shiyong; Liu, Zongwen
      Applied Clay Science (2018), 159 (), 102-106CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
      Methoxy-modified kaolinite was used as a novel carrier for anticancer drug 5-fluorouracil (5FU). The selective loading of 5FU into the interlayer space of methoxy-modified kaolinite was achieved because the weakly bonded 5FU on the external surface was removed off by facile water rinse. The intercalated 5FU has strong affinity (electrostatic force and hydrogen bonding) with the interlayer surface of kaolinite, and its release was controlled because of the diffusion restriction of the kaolinite lamellar layers and the strong affinity between 5FU and kaolinite. The controlled release of 5FU from methoxy-modified kaolinite in simulated colonic fluid (pH 5.5) makes it be of potential use to administer an oral formulation of 5FU for colon specific delivery.
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    27. 27
      Abukhadra, M. R.; Mohamed, A. S.; El-Sherbeeny, A. M.; Soliman, A. T. A. Enhanced Adsorption of Toxic and Biologically Active Levofloxacin Residuals from Wastewater Using Clay Nanotubes as a Novel Fixed Bed: Column Performance and Optimization. ACS Omega 2020, 5 (40), 26195– 26205,  DOI: 10.1021/acsomega.0c03785
      27
      Enhanced adsorption of toxic and biologically active levofloxacin residuals from wastewater using clay nanotubes as a novel fixed bed: Column performance and optimization
      Abukhadra, Mostafa R.; Mohamed, Aya S.; El-Sherbeeny, Ahmed M.; Soliman, Ahmed Tawhid Ahmed
      ACS Omega (2020), 5 (40), 26195-26205CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      Kaolinite nanotube particles (KNTs) were synthesized by a chem. exfoliation and scrolling process in the existence of sonication waves. The KNT product was identified as a mesoporous material (12 nm in pore diam.) with high surface area (105 m2/g) and promising adsorption affinity for the levofloxacin antibiotic (LVOX) residuals in wastewater. The KNT particles were used as a fixed bed in the continuous adsorption column system for LVOX considering the essential variables. The investigation of the KNT fixed bed in a continuous column for 1800 min verified its suitability to reduce the LVOX content in 9 L of polluted solns. by 80.4%. This was recognized after using the KNT bed of 4 cm in height, a flow rate of 5 mL/min, a pH value of 8, a total flow interval of 1800 min, and an LVOX concn. of 10 mg/L. The regeneration study of the bed declared effective recyclability properties for the KNT particles in the LVOX adsorption column system. The dynamic properties of the KNT bed-based column system were explained based on Thomas, Adams-Bohart, and the Yoon-Nelson kinetic models. The LVOX adsorption reaction by KNTs follows Langmuir behavior with homogeneous and monolayer uptake form. The Gaussian energy (2.05 kJ/mol) and the thermodn. parameters emphasized phys., spontaneous, and exothermic adsorption reactions for LVOX by KNTs.
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    28. 28
      Guha, A.; Chattoraj, S. L.; Chatterjee, S.; Kumar, K. V.; Rao, P. V. N.; Bhaumik, A. K. Reflectance Spectroscopy-Guided Broadband Spectral Derivative Approach to Detect Glauconite-Rich Zones in Fossiliferous Limestone, Kachchh Region, Gujarat, India. Ore Geol. Rev. 2020, 127, 103825  DOI: 10.1016/j.oregeorev.2020.103825
      There is no corresponding record for this reference.
    29. 29
      Bruneel, Y.; Van Laer, L.; Brassinnes, S.; Smolders, E. Characterisation of the Highly Selective Caesium Sorption on Glauconite Rich Sands of Contrasting Geological Formations. Appl. Geochem. 2021, 128, 104926  DOI: 10.1016/j.apgeochem.2021.104926
      29
      Characterisation of the highly selective caesium sorption on glauconite rich sands of contrasting geological formations
      Bruneel, Y.; Van Laer, L.; Brassinnes, S.; Smolders, E.
      Applied Geochemistry (2021), 128 (), 104926CODEN: APPGEY; ISSN:0883-2927. (Elsevier Ltd.)
      The Neogene-Paleogene glauconite sands are investigated in the framework of the Belgian radioactive waste disposal as material for an addnl. sorption sink. Glauconite is an Fe-rich phyllosilicate that is mainly present as 125-250 μm sized pellets in the sand. Recent studies have shown a surprisingly strong sorption of radiocaesium (137Cs) on these sands, despite the coarse sized pellet structure. This study was set up to characterize the selective 137Cs+ sorption sites on glauconite that are likely Frayed Edge Sites (FES) as in illite. First, the NH4/K selectivity on the FES was detd. as a fingerprint for the highly selective FES. The NH4/K selectivity coeff. on the FES for three different sand formation ranged between 3.8 and 5.0, well in line with the range (4-7) that has been reported for illite clay and clay formations. Second, the Cs+ sorption isotherms were detd. on three sand formations in a background soln. of 0.5 mM K+, 100 mM Ca+ and 10-8-10-4 M Cs+; isotherms were fitted with an optimized three-site model adapted after the illite model of Bradbury and Baeyens (2000). The optimized model fitted the data adequately. Taken together, this study suggests that the glauconite sands have highly selective sites that bind 137Cs+ with similar properties as in illite, however the fractions of these sites in the total CEC pool are about a factor five lower than in pure illite.
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    30. 30
      Singla, R.; Alex, T. C.; Kumar, R. On Mechanical Activation of Glauconite: Physicochemical Changes, Alterations in Cation Exchange Capacity and Mechanisms. Powder Technol. 2020, 360, 337– 351,  DOI: 10.1016/j.powtec.2019.10.035
      30
      On mechanical activation of glauconite: Physicochemical changes, alterations in cation exchange capacity and mechanisms
      Singla, Rashmi; Alex, Thomas C.; Kumar, Rakesh
      Powder Technology (2020), 360 (), 337-351CODEN: POTEBX; ISSN:0032-5910. (Elsevier B.V.)
      Mech. activation (MA) of glauconite [(K,Na,Ca)(Fe3+,Al,Mg,Fe2+)2(Si,Al)4O10(OH)2] has been investigated to improve its cation exchange capacity (CEC), an impediment for its direct use as nutrients (agro-mineral), notably potassium. Glauconite is mech. activated using planetary ball milling for varying lengths of time up to 240 min. Milling induces time dependent physicochem. changes in terms of particulate characteristics (morphol., particles size distribution, geometrical and BET sp. surface area), structure (crystallite size and strain; -OH/H2O bonding) and surface charge (zeta potential). It is possible to tailor the CEC of glauconite with MA. A remarkable improvement (30-fold!) in the CEC of K+ ions is possible. The effect of milling time on the exchange behavior is ion-specific. Plausible mechanisms of cation exchange are presented in terms of the chem. nature of the ions involved and the physicochem. changes. Lastly, MA approach is compared with reported methods of potassium recovery; its superiority as a green option is underlined.
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    31. 31
      Shmandiy, V.; Rigas, T.; Kharlamova, O.; Bezdeneznych, L. Research of Adsorption Properties of Glauconite-Based Composite Adsorbents. Journal of Ecological Engineering 2020, 21 (6), 147– 154,  DOI: 10.12911/22998993/123245
      There is no corresponding record for this reference.
    32. 32
      Abukhadra, M. R.; Bakry, B. M.; Adlii, A.; Yakout, S. M.; El-Zaidy, M. E. Facile Conversion of Kaolinite into Clay Nanotubes (KNTs) of Enhanced Adsorption Properties for Toxic Heavy Metals (Zn2+, Cd2+, Pb2+, and Cr6+) from Water. Journal of Hazardous Materials 2019, 374, 296– 308,  DOI: 10.1016/j.jhazmat.2019.04.047
      32
      Facile conversion of kaolinite into clay nanotubes (KNTs) of enhanced adsorption properties for toxic heavy metals (Zn2+, Cd2+, Pb2+, and Cr6+) from water
      Abukhadra, Mostafa R.; Bakry, Belal Mohamed; Adlii, Alyaa; Yakout, Sobhy M.; El-Zaidy, Mohamed A.
      Journal of Hazardous Materials (2019), 374 (), 296-308CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
      Kaolinite nanotubes (KNTs) were synthesized from kaolinite by ultrasonic scrolling and characterized using X-ray diffractometer, scanning and transmission electron microscopes; and FTIR-FT Raman spectrometer. The synthetic KNTs appear as multi-walled scrolls of 12 nm av. pore diam. and 50-600 nm particle length; and exhibit surface area of 105 m2/g. KNTs were used as adsorbents for Zn2+, Cd2+, Pb2+, and Cr6+ with uptake capacities of 103 mg/g, 116 mg/g, 89 mg/g, and 91 mg/g, resp. The equilibration time of Cd2+ and Pb2+ adsorption is 360 min and for Cr6+ and Zn2+ area 120 min and 240 min, resp. KNTs adsorption systems can be described mainly by Lagergren-second order and Freundlich models (R2> 0.95) as kinetic and isotherm models. This reflected multilayer adsorption forms with chem. sharing or ion exchange processes. KNTs exhibits high reusability and used for five cycles in the removal of the studied metals (100 mg/L). The removal percentages declined by 20.5%, 15.12%, 22.8% and 23.16% with repeating the reused cycles from cycle 1 to cycle 5 for Zn2+, Cd2+, Pb2+, and Cr6+, resp. KNTs were applied successfully in realistic purifn. of tap water, groundwater, and sewage water from the inspected metals.
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    33. 33
      Franus; Bandura; Madej Mono and Poly-Cationic Adsorption of Heavy Metals Using Natural Glauconite. Minerals 2019, 9 (8), 470,  DOI: 10.3390/min9080470
      33
      Mono and poly-cationic adsorption of heavy metals using natural glauconite
      Franus, Malgorzata; Bandura, Lidia; Madej, Jaroslaw
      Minerals (Basel, Switzerland) (2019), 9 (8), 470CODEN: MBSIBI; ISSN:2075-163X. (MDPI AG)
      The issue of heavy metal pollution of industrial wastewaters is a major environmental concern nowadays. The aim of this study was to investigate the effectiveness of heavy metals removal from aq. solns. by natural glauconite, in batch and dynamic systems. Glauconite was characterized by X-ray diffraction, nitrogen adsorption-desorption isotherm, scanning electron microscope, DTA, and inductively coupled plasma spectroscopy. Cation exchange capacity, bulk d. and point of zero charge were also detd. In the batch system, the impact of initial concn., contact time, and pH of metal solns. on sorption efficiency was analyzed, whereas for the dynamic system, the influence of flow rate was studied. The adsorption capacity in the batch system followed the order: Pb > Cd > Zn > Cu. The highest adsorption rate was achieved in the pH range 7-9. In the column expts., the selectivity order in the case of mono-cationic system was the same as that of batch system, whereas in the case of poly-cationic system it was: Pb > Zn > Cd > Cu. With the increase of the flow rate, the total capacity at the exhaustion point increased.
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    34. 34
      Baldermann, A.; Banerjee, S.; Czuppon, G.; Dietzel, M.; Farkaš, J.; Löhr, S.; Moser, U.; Scheiblhofer, E.; Wright, N. M.; Zack, T. Impact of Green Clay Authigenesis on Element Sequestration in Marine Settings. Nat. Commun. 2022, 13 (1), 1527,  DOI: 10.1038/s41467-022-29223-6
      34
      Impact of green clay authigenesis on element sequestration in marine settings
      Baldermann, Andre; Banerjee, Santanu; Czuppon, Gyoergy; Dietzel, Martin; Farkas, Juraj; Lohr, Stefan; Moser, Ulrike; Scheiblhofer, Esther; Wright, Nicky M.; Zack, Thomas
      Nature Communications (2022), 13 (1), 1527CODEN: NCAOBW; ISSN:2041-1723. (Nature Portfolio)
      Retrograde clay mineral reactions (reverse weathering), including glauconite formation, are first-order controls on element sequestration in marine sediments. Here, we report substantial element sequestration by glauconite formation in shallow marine settings from the Triassic to the Holocene, averaging 3 ± 2 mmol·cm-2·kyr-1 for K, Mg and Al, 16 ± 9 mmol·cm-2·kyr-1 for Si and 6 ± 3 mmol·cm-2·kyr-1 for Fe, which is ≈2 orders of magnitude higher than ests. for deep-sea settings. Upscaling of glauconite abundances in shallow-water (0-200 m) environments predicts a present-day global uptake of ≈≤ 0.1 Tmol·yr-1 of K, Mg and Al, and ≈0.1-0.4 Tmol·yr-1 of Fe and Si, which is ≈half of the estd. Mesozoic elemental flux. Clay mineral authigenesis had a large impact on the global marine element cycles throughout Earth's history, in particular during 'greenhouse' periods with sea level highstand, and is key for better understanding past and present geochem. cycling in marine sediments.
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    35. 35
      Pietsch, C.; Harrison, H. C.; Allmon, W. D. Whence the Gosport Sand (Upper Middle Eocene, Alabama)? The Origin of Glauconitic Shell Beds In the Paleogene of the U.S. Gulf Coastal Plain. Journal of Sedimentary Research 2016, 86 (11), 1249– 1268,  DOI: 10.2110/jsr.2016.72
      35
      Whence the gosport sand (Upper Middle Eocene, Alabama)? The oriign of glauconitic shell beds in the paleogene of the U.S. Gulf Coastal Plain
      Pietsch, Carlie; Harrison, H. Cliff; Allmon, Warren D.
      Journal of Sedimentary Research (2016), 86 (11), 1249-1268CODEN: JSERFV; ISSN:1938-3681. (SEPM Society for Sedimentary Geology)
      An explanation for the depositional history of the Gosport Sand has proven to be as puzzling as its diverse mollusk fossils is beguiling. We propose that shifting delta lobes produced patchy environments which accumulated to form the Gosport Sand and likely other glauconite- and fossil-rich shell beds of the Gulf Coastal Plain of the Paleogene. We present facies and mineralogical data to suggest glauconite in the Gosport Sand was deposited during relatively stable environmental conditions. Increased glauconite maturity and taphonomic alteration in the Gosport Sand are attributed to eustatic transgression, resulting in decreased deposition, enhanced winnowing, and increased exposure at the sediment-water interface. Increased fossil diversity and abundance likely result from time averaging and accumulation of shells from ancient patchy habitats analogous to modern "inner shallow shelf" and "open sound" environments. Delta progradation and subsidence would have detd. the migration of these environments. We evoke a similar depositional model for glauconite-rich shell beds distributed throughout the Paleocene and Eocene of the Gulf Coastal Plain based on their transgressive nature and roughly equiv. facies. These shifting environmental conditions may have played a partial role in generating the high molluscan diversity of the Gulf Coastal Plain of the Paleogene.
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    36. 36
      El-Habaak, G.; Askalany, M.; Faraghaly, M.; Abdel-Hakeem, M. The Economic Potential of El-Gedida Glauconite Deposits, El-Bahariya Oasis, Western Desert. Egypt. Journal of African Earth Sciences 2016, 120, 186– 197,  DOI: 10.1016/j.jafrearsci.2016.05.007
      There is no corresponding record for this reference.
    37. 37
      Sobeih, M. M.; El-Shahat, M. F.; Osman, A.; Zaid, M. A.; Nassar, M. Y. Glauconite Clay-Functionalized Chitosan Nanocomposites for Efficient Adsorptive Removal of Fluoride Ions from Polluted Aqueous Solutions. RSC Adv. 2020, 10 (43), 25567– 25585,  DOI: 10.1039/D0RA02340J
      37
      Glauconite clay-functionalized chitosan nanocomposites for efficient adsorptive removal of fluoride ions from polluted aqueous solutions
      Sobeih, Marwa M.; El-Shahat, M. F.; Osman, A.; Zaid, M. A.; Nassar, Mostafa Y.
      RSC Advances (2020), 10 (43), 25567-25585CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
      We herein have developed a mild approach for the fabrication of glauconite clay (G)-modified chitosan (CS) nanocomposites by the combination of a simple blending and crosslinking method. The chitosan was modified with EDTA (EDTA), glutaraldehyde (GL), sodium dodecyl sulfate (SDS), and cetyltrimethyl ammonium bromide (CTAB). The as-prepd. composites were identified using Fourier-transform IR spectroscopy (FTIR), X-ray diffraction (XRD), field emission SEM (FE-SEM), nitrogen phys. adsorption (BET), at. absorption spectrophotometry (AA), and thermal gravimetric anal. (TGA). The adsorption activities of the as-prepd. materials were assessed for the removal of fluoride ions from aq. media using a batch technique. Raw glauconite (G), GL-CS/G, SDS-CS/G, EDTA-GL-CS/G, and CTAB-CS/G adsorbents displayed max. adsorption capacity values of 1.15, 4.31, 4.55, 6.90, and 9.03 mg g-1, resp. The adsorption results were well described by employing the pseudo-second-order kinetic and Langmuir isotherm models. The estd. thermodn. consts. indicated that the F- ion adsorption was a spontaneous, physisorption process. Furthermore, the modified chitosan adsorbents are good candidates for the adsorptive elimination of F- ions from aq. solns., according to their reusability, high stability, good adsorption capacity, and applicability for actual field water samples.
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    38. 38
      Moretto, L. M.; Orsega, E. F.; Mazzocchin, G. A. Spectroscopic Methods for the Analysis of Celadonite and Glauconite in Roman Green Wall Paintings. Journal of Cultural Heritage 2011, 12 (4), 384– 391,  DOI: 10.1016/j.culher.2011.04.003
      There is no corresponding record for this reference.
    39. 39
      Shawky, A.; El-Sheikh, S. M.; Rashed, M. N.; Abdo, S. M.; El-Dosoqy, T. I. Exfoliated Kaolinite Nanolayers as an Alternative Photocatalyst with Superb Activity. Journal of Environmental Chemical Engineering 2019, 7 (3), 103174  DOI: 10.1016/j.jece.2019.103174
      39
      Exfoliated kaolinite nanolayers as an alternative photocatalyst with superb activity
      Shawky, Ahmed; El-Sheikh, Said M.; Rashed, Mohamed Nageeb; Abdo, Sabrin M.; El-Dosoqy, Thanaa I.
      Journal of Environmental Chemical Engineering (2019), 7 (3), 103174CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
      In searching for alternative and abundant photocatalyst, exfoliated kaolinite nanolayers (nK) were prepd. by a simple intercalation process. The effect of intercalating agents on the produced nK was studied by different instrumentations. XRD, FT-IR, and TEM confirm the exfoliation of kaolinite into nanolayers. Bandgap values were altered depending on intercalating agents as revealed by light absorption spectra. Photogenerated charge carriers obsd. through photoluminescence spectra. The produced nK applied for photodegrdn. of Rhodamine B dye (RhB) as an industrial model for wastewater treatment purposes. The results showed a complete photodegrdn. of RhB within a few minutes under UV with superb reaction kinetics. We refer the enhanced photocatalytic properties to the exposed metal oxide impurities on the surface of nK due to exfoliation. Performance tests revealed the reusability and stability of the prepd. nK. This plentiful material is supposed to be a versatile alternative for the well-known photocatalysts with the possibility of large-scale prodn. Photodegrdn. mechanism of RhB is proposed.
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    40. 40
      Younes, H.; El-Etriby, H. Kh.; Mahanna, H. High Removal Efficiency of Reactive Yellow 160 Dye from Textile Wastewater Using Natural and Modified Glauconite. International Journal of Environmental Science and Technology 2022, 19 (6), 5659– 5674,  DOI: 10.1007/s13762-021-03528-3
      40
      High removal efficiency of reactive yellow 160 dye from textile wastewater using natural and modified glauconite
      Younes, H.; El-Etriby, H. Kh.; Mahanna, H.
      International Journal of Environmental Science and Technology (2022), 19 (6), 5659-5674CODEN: IJESHU; ISSN:1735-1472. (Springer)
      The adsorption of reactive yellow 160 (RY160) dye from textile wastewater was investigated using natural clay glauconite as an eco-friendly and low-cost adsorbent. Besides, modifications methods by thermal activation (TAG) and acid activation (AAG) of glauconite were studied to enhance the removal efficiency and adsorption capacity. Glauconite samples were characterized by FTIR spectroscopy, XRD, SEM, EDX, nitrogen adsorption/desorption isotherm, and zeta potential. Moreover, the effect of initial concn., contact time, adsorbent dose, pH, and temp. on the removal efficiency was studied. The results show that RY160 removal efficiency increases by increasing adsorbent dose. The removal efficiency reached 92.32% by raw glauconite and 100% by modified glauconite at a dose of 4 g/L. The max. adsorption of the RY160 dye is detected at pH 1.0 for raw and modified glauconite. The adsorption of RY160 on glauconite is exothermic and spontaneous. The isotherm study revealed that Freundlich isotherm fits well the exptl. data. The max. adsorption capacity improved from 29.85 mg/g for raw glauconite to 51.55 and 55.87 mg/g for TAG, and AAG, resp. The pseudo-second-order model well expresses the exptl. data (R2 = 0.997). The reusability study showed that the adsorbents could effectively regenerated and reused. The results imply that the modified glauconite could be used as a natural and low-cost adsorbent for RY160 dye removal from textile wastewater.
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    41. 41
      Salam, M. A.; Abukhadra, M. R.; Mostafa, M. Effective Decontamination of As(V), Hg(II), and U(VI) Toxic Ions from Water Using Novel Muscovite/Zeolite Aluminosilicate Composite: Adsorption Behavior and Mechanism. Environmental Science and Pollution Research 2020, 27 (12), 13247– 13260,  DOI: 10.1007/s11356-020-07945-8
      41
      Effective decontamination of As(V), Hg(II), and U(VI) toxic ions from water using novel muscovite/zeolite aluminosilicate composite: adsorption behavior and mechanism
      Salam, Mohamed Abdel; Abukhadra, Mostafa R.; Mostafa, Merna
      Environmental Science and Pollution Research (2020), 27 (12), 13247-13260CODEN: ESPLEC; ISSN:0944-1344. (Springer)
      Muscovite/phillipsitic zeolite was introduced as a novel inorg. composite of stunning adsorption properties. The composite was investigated in the uptake reactions of Hg(II), As(V), and U(VI) as highly toxic water contaminants considering different adsorption factors. The adsorption properties of muscovite/phillipsitic zeolite are highly dependent on the pH values and the best decontamination percentages can be obtained at pH 4, pH 5, and pH 5 for Hg(II), As(V), and U(VI), resp. The kinetic studies demonstrated adsorption equil. for Hg(II), As(V), and U(VI) after 360 min, 300 min, and 360 min, resp. The equil. modeling suggested monolayer uptake for all the metals and represented mainly by the Langmuir model considering both the values of detn. coeff. and chi-squared (χ2). The estd. max. capacities are 117 mg/g (Hg(II)), 122.5 mg/g (As(V)), and 138.5 mg/g (U(VI)) which are higher values than several studied adsorbents. The Dubinin-Radushkevich adsorption energies of Hg(II) (19.4 kJ/mol), As(V) (25.6 kJ/mol), and U(VI) (26.47 kJ/mol) signify chem. adsorption mechanisms and close to the obtained values for the ion-exchange process. Addnl., the composite is of high reusability properties and was applied effectively for five decontamination cycles.
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    42. 42
      Kumar, U.; Bandayopadhyay, M. Sorption of Cadmium from Aqueous Solution Using Pretreated Rice Husk. Bioresour. Technol. 2006, 97 (1), 104– 109,  DOI: 10.1016/j.biortech.2005.02.027
      42
      Sorption of cadmium from aqueous solution using pretreated rice husk
      Kumar Upendra; Bandyopadhyay Manas
      Bioresource technology (2006), 97 (1), 104-9 ISSN:0960-8524.
      The sorption of Cd(II) from aqueous solution by rice husk, a surplus agricultural byproduct was investigated. Some simple and low-cost chemical modifications resulted in increasing the sorption capacity of raw rice husk (RRH) from 8.58 mg/g to 11.12, 20.24, 16.18 mg/g and reducing the equilibrium time from 10 h of RRH to 2, 4 and 1 h for epichlorohydrin treated rice husk (ERH), NaOH treated rice husk (NRH), sodium bicarbonate treated rice husk (NCRH), respectively. The effect of pH, sorption kinetics and isotherms were studied in batch experiments. Good correlation coefficient was obtained for pseudo second-order kinetic model, which agreed with chemisorption as the rate-limiting mechanism. Sorption isotherm test showed that equilibrium sorption data were better represented by Langmuir model than the Freundlich model. The highly efficient low cost and the rapid uptake of Cd(II) by NCRH indicated that it could be an excellent alternative for the removal of heavy metal by sorption process.
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    43. 43
      Yuan, P.; Tan, D.; Annabi-Bergaya, F.; Yan, W.; Liu, D.; Liu, Z. From Platy Kaolinite to Aluminosilicate Nanoroll via One-Step Delamination of Kaolinite: Effect of the Temperature of Intercalation. Appl. Clay Sci. 2013, 83–84, 68– 76,  DOI: 10.1016/j.clay.2013.08.027
      43
      From platy kaolinite to aluminosilicate nanoroll via one-step delamination of kaolinite: Effect of the temperature of intercalation
      Yuan, Peng; Tan, Daoyong; Annabi-Bergaya, Faiza; Yan, Wenchang; Liu, Dong; Liu, Zongwen
      Applied Clay Science (2013), 83-84 (), 68-76CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
      Aluminosilicate nanorolls were prepd. using a method of one-step delamination of kaolinite. In this method, cetyltrimethylammonium chloride (CTMACl) was intercalated into the interlayer space of methoxy-modified kaolinite, which resulted in the delamination and rolling of kaolinite layers. The reaction conditions of CTMACl intercalation significantly influenced the formation of nanorolls, as shown by characterizations using X-ray diffraction, electron microscopy, IR spectroscopy, thermal anal., and nitrogen adsorption. Overall, increasing the CTMACl-intercalation temp. helps to promote the transformation from platy kaolinite to nanorolls. The initial kaolinite particles were mostly transformed to nanorolls in the product prepd. at 80 !!!C, whereas considerable kaolinite particles remained untransformed in the product prepd. at 30 !!!C. At 80 !!!C, the obtained sp. surface area (SSA) and the porous vol. (Vpor) values of the nanoroll product are nearly twice the values obtained at 30 !!!C and the tubular structure exhibits higher thermal persistence. The tubular morphol. and the porosity of these nanorolls obtained at 80 !!!C, were largely retained after calcination at 600-800 !!!C. However, a calcination at 900 !!!C led to an obvious distortion of the nanorolls and a decrease in SSA and Vpor values. The obsd. structural changes of the nanorolls under calcination generally resembled that of natural halloysite but occurred at lower temps. because the prepd. nanorolls were of lower structural order with thinner tube walls.
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    44. 44
      Vivas, E. L.; Cho, K. Efficient Adsorptive Removal of Cobalt(II) Ions from Water by Dicalcium Phosphate Dihydrate. Journal of Environmental Management 2021, 283, 111990  DOI: 10.1016/j.jenvman.2021.111990
      44
      Efficient adsorptive removal of Cobalt(II) ions from water by dicalcium phosphate dihydrate
      Vivas, Eleazer L.; Cho, Kuk
      Journal of Environmental Management (2021), 283 (), 111990CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
      Although the radionuclide 60Co is widely used, its presence in various effluents demands its removal to preclude environmental pollution and detrimental effects on human health. This study investigated the batch adsorption performance of a potential cobalt adsorbent, dicalcium phosphate dihydrate (DCPD), in immobilizing Co2+ from water. The influences of soln. pH, contact time, initial concn., and competing cations were examd. and discussed. Stable cobalt uptake was obsd. at pH 4-8. The sorption kinetics showed a multi-stage uptake profile, implying that several mechanisms are involved in the adsorption process. Microscopy and structural anal. revealed that DCPD decomps. to its anhyd. form during adsorption, which explains the multistep curve over the entire adsorption period. However, the non-apatitic transformation is not exclusive to cobalt uptake. Intraparticle diffusion also contributed to the overall removal kinetics of Co2+ from water. Considering the Sips isotherm model, the max. Co2+ adsorption capacity of DCPD was 441 mg g-1. Cobalt uptake selectivity dropped in the presence of Ca2+ ions, from 1.21 x 104 to 207 mL g-1, indicating DCPD would be more applicable in treating soft 60Co-contaminated waters. Structural anal., elemental mapping, and qual. anal. of solid residues confirmed that ion exchange is involved in the removal of cobalt from aq. solns.
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    45. 45
      El-Zahhar, A. A.; Awwad, N. S. Removal of Malachite Green Dye from Aqueous Solutions Using Organically Modified Hydroxyapatite. Journal of Environmental Chemical Engineering 2016, 4 (1), 633– 638,  DOI: 10.1016/j.jece.2015.12.014
      45
      Removal of malachite green dye from aqueous solutions using organically modified hydroxyapatite
      El-Zahhar, Adel A.; Awwad, Nasser S.
      Journal of Environmental Chemical Engineering (2016), 4 (1), 633-638CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
      The removal of malachite green dye (MG) from aq. soln. was studied using organically modified hydroxyapatite. Hydroxyapatite (HAP) was organically modified with different concns. of the org. surfactant ethylhexadecyldimethyl ammonium bromide (EHDAB). The modified apatite was characterized using FTIR, XRD and SEM. The modified apatite was studied for removal of MG from aq. soln. and the exptl. parameters were studied. The effect of contact time, adsorbent dose, dye concn. and temp. was studied. The equil. uptake was increased with increasing the initial dye concn. in soln. The exptl. isotherm data were analyzed using Langmuir adsorption isotherm model. The adsorbed amt. of MG onto the modified apatite was found to increase with increasing the adsorbent concn. The max. monolayer adsorption capacity was found to be 188.18 mg/g at 30°C.
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    46. 46
      Zhang, F.; Ma, B.; Jiang, X.; Ji, Y. Dual Function Magnetic Hydroxyapatite Nanopowder for Removal of Malachite Green and Congo Red from Aqueous Solution. Powder Technol. 2016, 302, 207– 214,  DOI: 10.1016/j.powtec.2016.08.044
      46
      Dual function magnetic hydroxyapatite nanopowder for removal of malachite green and Congo red from aqueous solution
      Zhang, Fan; Ma, Baoliang; Jiang, Xiping; Ji, Yuefei
      Powder Technology (2016), 302 (), 207-214CODEN: POTEBX; ISSN:0032-5910. (Elsevier B.V.)
      In this study, the removal of both cationic dye (malachite green) and anionic dye (Congo red) by magnetic Sr5xBa3x(PO4)3(OH)/Fe3O4 nanopowder (namely SBPF) from aq. soln. was investigated. Variables influencing the adsorption capacity, such as soln. pH, temp., adsorbent dosage, adsorption time, and initial concn., were systematically investigated. The adsorption process is pH and temp. dependent. The adsorption for MG and CR can be described by pseudo-first-order and pseudo-second-order kinetic model, resp. The adsorption behaviors fit quite well with the Langmuir model for both dyes with the max. adsorption capacity of 526 mg g-1 for MG and 417 mg g-1 for CR. Thermodn. anal. revealed that the adsorption processes were spontaneous and exothermic. Phys. forces, hydrogen bonding, and ionic interaction are responsible for binding of the dyes with SBPF. The used SBPF nanopowder could be regenerated effectively and recycled for five cycles without a significant loss of adsorption ability. Moreover, the adsorbent can be applied to remove MG and CR in different water matrixes.
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    47. 47
      Lee, Y.-C.; Kim, J.-Y.; Shin, H.-J. Removal of Malachite Green (MG) From Aqueous Solutions by Adsorption, Precipitation, and Alkaline Fading Using Talc. Sep. Sci. Technol. 2013, 48 (7), 1093– 1101,  DOI: 10.1080/01496395.2012.723100
      47
      Removal of Malachite Green (MG) From Aqueous Solutions by Adsorption, Precipitation, and Alkaline Fading Using Talc
      Lee, Young-Chul; Kim, Jin-Young; Shin, Hyun-Jae
      Separation Science and Technology (Philadelphia, PA, United States) (2013), 48 (7), 1093-1101CODEN: SSTEDS; ISSN:0149-6395. (Taylor & Francis, Inc.)
      Malachite Green (MG), which is primarily used as a dye, is a chem. that is listed as a class II health hazard because of its toxicity to humans and the environment. Adsorption is frequently used to remove this cationic dye from aq. solns. Structural changes of the mol. should be considered during removal, because MG (or chromatic MG+ at neutral pH) turns into protonated MG (MGH+) at acidic pHs and a carbinol base at basic pHs. Batch sorption expts. were conducted to remove MG from aq. solns. using talc. We studied specific removal behaviors and mechanisms of the MG for different pH solns., including adsorption, pptn., and alk. fading.
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    48. 48
      Chen, Y.; Nie, Z.; Gao, J.; Wang, J.; Cai, M. A Novel Adsorbent of Bentonite Modified Chitosan-Microcrystalline Cellulose Aerogel Prepared by Bidirectional Regeneration Strategy for Pb(II) Removal. Journal of Environmental Chemical Engineering 2021, 9 (4), 105755  DOI: 10.1016/j.jece.2021.105755
      48
      A novel adsorbent of bentonite modified chitosan-microcrystalline cellulose aerogel prepared by bidirectional regeneration strategy for Pb(II) removal
      Chen, Yan; Nie, Zeguang; Gao, Junkai; Wang, Jiaqi; Cai, Miaomiao
      Journal of Environmental Chemical Engineering (2021), 9 (4), 105755CODEN: JECEBG; ISSN:2213-3437. (Elsevier Ltd.)
      Traditional chitosan aerogel (CSA) could be used to chelate heavy metal ions due to its large sp. surface area, high porosity and rich amino groups. However, the CSA was rarely applied in practical application because of its easy hydrolysis, low mech. strength and slow adsorption rate. In this study, we developed a novel method for increasing the anti-hydrolytic ability and mech. strength of CSA by bidirectional regeneration of chitosan and microcryst. cellulose to synthesize chitosan-microcryst. cellulose aerogel (CS-MCCA). In addn., bentonite (BT) was introduced in the regeneration process to enhance the adsorption rate of CSA, and an efficient adsorbent of bentonite-chitosan-microcryst. cellulose aerogel (BT-CS-MCCA) for Pb(II) removal was developed, and the max. adsorption amt. and adsorption equil. time of Pb(II) on BT-CS-MCCA were 256.24 mg g-1 and 60 min, resp. Addnl., it was found that with the increase of Na+ or K+ concn. in the soln. from 0 mol L-1 to 0.1 mol L-1, the adsorption capacity of BT-CS-MCCA was enhanced, because the Ca2+ in BT was substituted by Na+ or K+ , and then the ion-exchange ability of BT-CS-MCCA was improved. Moreover, the prepn. method of BT-CS-MCCA possessed merits of simple operation, low cost and hypotoxicity. Thus, the BT-CS-MCCA had a broad potential application for the purifn. of Pb(II) in wastewater, and the bidirectional regeneration strategy might offer a brand-new path for the utilization of biomass resources.
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    49. 49
      Tran, T. N.; Do, Q. C.; Kim, D.; Kim, J.; Kang, S. Urchin-like Structured Magnetic Hydroxyapatite for the Selective Separation of Cerium Ions from Aqueous Solutions. Journal of Hazardous Materials 2022, 430, 128488  DOI: 10.1016/j.jhazmat.2022.128488
      49
      Urchin-like structured magnetic hydroxyapatite for the selective separation of cerium ions from aqueous solutions
      Tran, Thi Nhung; Do, Quoc Cuong; Kim, Dogun; Kim, Junho; Kang, Seoktae
      Journal of Hazardous Materials (2022), 430 (), 128488CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
      In this study, bio-inspired urchin-like structured hydroxyapatite (UHdA) and its magnetic composite (UHdA@Fe3O4) were developed for efficient and easy sepn. of cerium ions (Ce3+) from aquatic waste streams. UHdA and UHdA@Fe3O4 exhibited superior Ce3+ adsorption capacities of 248.39 and 230.01 mg/g-UHdA resp., compared to a com. HdA (141.71 mg/g-HdA) due to their hierarchical mesoporous structure and large sp. surface area. The adsorption of Ce3+ to UHdA and UHdA@Fe3O4 were heterogeneous, pseudo-second-order-kinetic, and the rate-limiting step was external mass transfer and intra-particle diffusion. Moreover, thermodn. studies revealed that the adsorption process was spontaneous and endothermic nature. The high selectivity towards Ce3+ in multi-ionic systems is attributed to the strong affinity between strong Lewis acid (Ce3+) and base (PO3-4 and OH-) interactions. XRD, FTIR, and XPS anal. demonstrated that the adsorption was mainly attributable to the ion exchange of Ce3+ with Ca2+ and to surface complexation. The desorption of Ce3+ was efficiently accomplished using 0.1 M HNO3. The results suggest that UHdA and UHdA@Fe3O4 could be promising choices for the adsorption and recovery of rare earth elements.
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    50. 50
      El Qada, E. Kinetic Behavior of the Adsorption of Malachite Green UsingJordanian Diatomite as Adsorbent. JORDANIAN JOURNAL OF ENGINEERING AND CHEMICAL INDUSTRIES (JJECI) 2020, 3 (1), 1– 10,  DOI: 10.48103/jjeci3120220
      There is no corresponding record for this reference.
    51. 51
      Lin, X.; Xie, Y.; Lu, H.; Xin, Y.; Altaf, R.; Zhu, S.; Liu, D. Facile Preparation of Dual La-Zr Modified Magnetite Adsorbents for Efficient and Selective Phosphorus Recovery. Chemical Engineering Journal 2021, 413, 127530  DOI: 10.1016/j.cej.2020.127530
      51
      Facile preparation of dual La-Zr modified magnetite adsorbents for efficient and selective phosphorus recovery
      Lin, Xiaochang; Xie, Yinglong; Lu, Huijie; Xin, Yicong; Altaf, Rubina; Zhu, Songming; Liu, Dezhao
      Chemical Engineering Journal (Amsterdam, Netherlands) (2021), 413 (), 127530CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
      Phosphate (P) is an irreplaceable resource for the growth of all living organisms, and the impending exhaustion of minable P rock arouses the demand of P recovery, which further promotes the novel technologies development. To reclaim the P from wastewater or sludge conveniently and efficiently, a novel magnetic adsorbent with La-Zr bimetallic modification (La-Zr@Fe3O4) possessing a high affinity to phosphate and rapid sepn. was proposed in this study. Adsorption tests showed that the adsorption capacity of P on La-Zr@Fe3O4 increased with La content, reaching the max. value of 49.3 mg/g at pH 3 by L1Z2. Whereas, the addn. of La resulted in the decline of desorption efficiency from ∼85% to ∼60% in the pH range from 3 to 6, except pH 2. The kinetics of P adsorption on the La-Zr@Fe3O4 was described well by the pseudo-second-order model, while the isotherm of P adsorption was fitted well by the Freundlich model. Besides, the adsorbent exhibited high selectivity towards P over other coexisting ions (Cl-, NO-3, SO2-4, Mg2+, and Ca2+). The feasibility of P recovery from the solid phase was investigated and confirmed by P recovery from fish farm sludge. The 90% removal efficiency of P and 88% desorption efficiency in cyclic adsorption/desorption expts. evidenced the stability and reusability of La-Zr magnetic adsorbent. The anal. of X-ray diffraction, Fourier transform IR spectrum, and XPS revealed the replacement of OH- with phosphate via the ligand exchange was the adsorption mechanism. This work demonstrated that the highly efficient, rapidly separable, and repeatable La-Zr@Fe3O4 has the potential for phosphate sequestration and recovery.
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    52. 52
      Jiang, Y.; Abukhadra, M. R.; Refay, N. M.; Sharaf, M. F.; El-Meligy, M. A.; Awwad, E. M. Synthesis of Chitosan/MCM-48 and β-Cyclodextrin/MCM-48 Composites as Bio-Adsorbents for Environmental Removal of Cd2+ Ions; Kinetic and Equilibrium Studies. React. Funct. Polym. 2020, 154, 104675  DOI: 10.1016/j.reactfunctpolym.2020.104675
      52
      Synthesis of chitosan/MCM-48 and β-cyclodextrin/MCM-48 composites as bio-adsorbents for environmental removal of Cd2+ ions; kinetic and equilibrium studies
      Jiang, Yuliang; Abukhadra, Mostafa R.; Refay, Nermen M.; Sharaf, Mohamed F.; El-Meligy, Mohammed A.; Awwad, Emad Mahrous
      Reactive & Functional Polymers (2020), 154 (), 104675CODEN: RFPOF6; ISSN:1381-5148. (Elsevier Ltd.)
      Chitosan/MCM-48 (CH/MCM) and β-cyclodextrin/MCM-48 (CD/MCM) composites were synthesized as promising and eco-friendly bio-adsorbents for Cd2+ ions from water. The composites showed novel porous structures and complex functional groups making them of high adsorption capacities. The adsorption behaviors of CH/MCM and CD/MCM are highly controlled by the tested pH values realizing their best capacities at pH 7. The kinetic evaluation indicated the excellent agreement between the uptake of Cd2+ by CH/MCM and CD/MCM with the pseudo-first-order model achieving equil. intervals of 480 min and 600 min, resp. Based on the values of Chi-squared (X2) and the correlation coeff., the composites displayed adsorption properties related to the Freundlich hypothesis with a multilayer form. Addnl., the Gaussian energies of them are 2.23 KJ/mol (CH/MCM) and 2.46 KJ/mol (CD/MCM) reflecting phys. uptake of Cd2+ by the studied composites. The thermodn. investigation implied spontaneous uptake of Cd2+ by the composites with endothermic reactions. The prepd. CH/MCM and CD/MCM are of 122.4 mg/g and 152.2 mg/g theor. qmax, resp. which are higher values than the reported results for several studied adsorbents. Moreover, the synthetic CH/MCM and CD/MCM showed high reusability as adsorbents for Cd2+ to be applied effectively six times.
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    53. 53
      Sherlala, A. I. A.; Raman, A. A. A.; Bello, M. M.; Buthiyappan, A. Adsorption of Arsenic Using Chitosan Magnetic Graphene Oxide Nanocomposite. Journal of Environmental Management 2019, 246, 547– 556,  DOI: 10.1016/j.jenvman.2019.05.117
      53
      Adsorption of arsenic using chitosan magnetic graphene oxide nanocomposite
      Sherlala, A. I. A.; Raman, A. A. A.; Bello, M. M.; Buthiyappan, A.
      Journal of Environmental Management (2019), 246 (), 547-556CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
      Chitosan-magnetic-graphene oxide (CMGO) nanocomposite was prepd. for arsenic adsorption. The nanocomposite was characterized through BET, FTIR, FESEM, EDX, and VSM analyses. These characterizations confirmed the formation of CMGO nanocomposites with high sp. surface area (152.38 m2/g) and excellent satn. magnetization (49.30 emu/g). Batch adsorption expts. were conducted to evaluate the performance of the nanocomposite in the adsorption of arsenic from aq. soln. The effects of operational parameters, adsorption kinetic, equil. isotherm and thermodn. were evaluated. The removal efficiency of arsenic increased with increasing adsorbent dosage and contact time. However, the effect of pH followed a different pattern, with the removal efficiency increasing from acidic to neutral pH, and then decreasing at alk. conditions. The highest adsorption capacity (45 mg/g) and removal efficiency (61%) were obtained at pH 7.3. The adsorption kinetic followed a pseudo-second-order kinetic model. The anal. of adsorption isotherm shows that the adsorption data fitted well to Langmuir isotherm model, indicating a homogeneous process. Thermodn. anal. shows that the adsorption of As(III) is exothermic and spontaneous. The superparamagnetic properties of the nanocomposite enabled the sepn. and recovery of the nanoparticles using an external magnetic field. Thus, the developed nanocomposite has a potential for arsenic remediation.
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    54. 54
      Huang, Y.; Zeng, X.; Guo, L.; Lan, J.; Zhang, L.; Cao, D. Heavy Metal Ion Removal of Wastewater by Zeolite-Imidazolate Frameworks. Sep. Purif. Technol. 2018, 194, 462– 469,  DOI: 10.1016/j.seppur.2017.11.068
      54
      Heavy metal ion removal of wastewater by zeolite-imidazolate frameworks
      Huang, Yan; Zeng, Xiaofei; Guo, Lingling; Lan, Jianhui; Zhang, Liangliang; Cao, Dapeng
      Separation and Purification Technology (2018), 194 (), 462-469CODEN: SPUTFP; ISSN:1383-5866. (Elsevier B.V.)
      With the rapid development of industrialization, removing heavy metal ions of wastewater from the discharge of industrial sewage is a very important topic, because it will severely affect our environment and water ecosystem. In this work, we synthesize two porous adsorbents of ZIF-8 and ZIF-67 and further investigate their performance of removing Pb2+ and Cu2+ from wastewater. Results indicate that satd. adsorption capacities of ZIF-8 and ZIF-67 for Pb2+ reach 1119.80 and 1348.42 mg/g, while they are 454.72 and 617.51 mg/g for Cu2+, resp., which are greatly higher than almost all other porous materials. If we use the excessive adsorbents to treat wastewater, more than 99.4% Pb2+ and 97.4% Cu2+ can be removed by ZIF-8 and ZIF-67 adsorbents. Moreover, the two adsorbents also show fast adsorption kinetics, and only need several decade minutes to reach adsorption equil. These features indicate that ZIF-8 and ZIF-67 are excellent candidates for removal of heavy metal ions from wastewater.
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    55. 55
      Jasper, E. E.; Ajibola, V. O.; Onwuka, J. C. Nonlinear Regression Analysis of the Sorption of Crystal Violet and Methylene Blue from Aqueous Solutions onto an Agro-Waste Derived Activated Carbon. Appl. Water Sci. 2020, 10 (6), 132,  DOI: 10.1007/s13201-020-01218-y
      55
      Nonlinear regression analysis of the sorption of crystal violet and methylene blue from aqueous solutions onto an agro-waste derived activated carbon
      Jasper, Enebi Estella; Ajibola, Victor Olatunji; Onwuka, Jude Chinedu
      Applied Water Science (2020), 10 (6), 132CODEN: AWSPCL; ISSN:2190-5495. (Springer GmbH)
      Abstr.: Sorption of synthetic dyes on low-cost solid sorbents is a simple technique for their removal from wastewater. This research investigates the sorption kinetics and equil. of two synthetic cationic dyes, crystal violet and methylene blue from aq. media using activated carbon prepd. from an agro-waste, Millettia thonningii seed pods. Sorption expts. were carried out using the batch process. The kinetic data were analyzed using the pseudo-first-order, pseudo-second-order, and intraparticle diffusion models while the equil. data were analyzed using the Langmuir, Freundlich, and Redlich-Peterson isotherm models. Nonlinear regression method was used to fit the data to the isotherm models in order to det. model parameters and the best-fit isotherms. Thus, three error functions; coeff. of detn., Chi-square statistic test, and the sum of error squares were applied to evaluate the sorption data. The pseudo-second-order model best described the sorption kinetics of both dyes while the Redlich-Peterson model described the equil. data the most, followed closely by the Freundlich isotherm model indicating a heterogeneous sorbent surface. The exptl. results indicate that the agro-waste derived activated carbon is a viable adsorbent for the remediation of dye-contaminated water.
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    56. 56
      Giles, C. H.; MacEwan, T. H.; Nakhwa, S. N.; Smith, D. 786. Studies in Adsorption. Part XI. A System of Classification of Solution Adsorption Isotherms, and Its Use in Diagnosis of Adsorption Mechanisms and in Measurement of Specific Surface Areas of Solids. Journal of the Chemical Society (Resumed) 1960, 3973,  DOI: 10.1039/jr9600003973
      There is no corresponding record for this reference.
    57. 57
      Abukhadra, M. R.; Dardir, F. M.; Shaban, M.; Ahmed, E. A.; Soliman, M. F. Superior Removal of Co2+, Cu2+ and Zn2+ Contaminants from Water Utilizing Spongy Ni/Fe Carbonate–Fluorapatite; Preparation, Application and Mechanism. Ecotoxicology and Environmental Safety 2018, 157, 358– 368,  DOI: 10.1016/j.ecoenv.2018.03.085
      57
      Superior removal of Co2+, Cu2+ and Zn2+ contaminants from water utilizing spongy Ni/Fe carbonate-fluorapatite; preparation, application and mechanism
      Abukhadra, Mostafa R.; Dardir, Fatma M.; Shaban, Mohamed; Ahmed, Ezzat A.; Soliman, Mamdouh F.
      Ecotoxicology and Environmental Safety (2018), 157 (), 358-368CODEN: EESADV; ISSN:0147-6513. (Elsevier B.V.)
      Spongy Ni/Fe carbonate - fluorapatite was synthesized from natural phosphorite enriched with iron impurities. The morphol., chem. and structural features of the product were estd. using several techniques as XRD, SEM, EDX, and FT-IR. It exhibits spongy structure of nano and micro-pores. The av. crystallite size is about 8.27nm. The suitability of the product for considerable decontamination of Zn2+, Co2+, and Cu2+, ions from water was studied based on several reacting parameters. The equil. was attained after 240min for Zn2+ and Co2+ ions while the adsorption equil. of Cu2+ reached after 120min. The adsorption data for the selected metals was represented well by a pseudo-second-order model which revealed chemisorption uptake. The equil. studies were appraised based on traditional models and two advanced models were designed according to the statistical phys. theories. The adsorption results highly fitted with Langmuir model followed rather than the other models. This indicated a monolayer adsorption for the metal ions by spongy Ni/Fe carbonate - fluorapatite. The estd. qmax values are 149.25mg/g, 106.4mg/g and 147.5mg/g for the uptake of Zn2+, Co2+, and Cu2+, resp. Based on monolayer models of one energy and two energies, the no. of receptor adsorption sites, no. of adsorbed metal ions per active site, the av. no. of sites which occupied by ions, mono layer adsorption quantity and the adsorption quantity after total satn. were calcd. for the first time for such materials.
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    58. 58
      Shaban, M.; Abukhadra, M. R.; Shahien, M. G.; Khan, A. A. P. Upgraded Modified Forms of Bituminous Coal for the Removal of Safranin-T Dye from Aqueous Solution. Environmental Science and Pollution Research 2017, 24 (22), 18135– 18151,  DOI: 10.1007/s11356-017-9424-4
      58
      Upgraded modified forms of bituminous coal for the removal of safranin-T dye from aqueous solution
      Shaban, Mohamed; Abukhadra, Mostafa R.; Shahien, Mohamed G.; Khan, Aftab Aslam Parwaz
      Environmental Science and Pollution Research (2017), 24 (22), 18135-18151CODEN: ESPLEC; ISSN:0944-1344. (Springer)
      Natural bituminous coal was used as a precursor in the synthesis of different modified products. The modification of coal was performed by treating it with nitric acid (N-coal), coating its surface by zinc oxide nanoparticles (Z-coal), and converting it into porous graphite (PG). The effect of modification processes on the structures, morphologies, and optical properties was followed by X-ray diffraction (XRD), SEM (SEM), Fourier transform IR spectrum (FT-IR), and UV/VIS spectrophotometer anal. The surface of N-coal grains becomes smoother than the surface of raw coal grains due to the removal of the assocd. impurities and the formation of nitrogen function groups. For Z-coal, the whole surface of coal grains appears to be completely covered by agglomerated ZnO nanoparticles of massive d. and irregular shapes. The av. crystallite size of the formed ZnO is ∼22.2 nm and d. of dislocations is 2.029 × 10-3 dislocation/nm2. Also, the removal of safranin-T dye by natural bituminous coal and its modified forms was investigated as a function of contact time, adsorbent mass, initial dye concn., and pH value. The obtained results are well fitted by pseudo-second-order kinetic than by intraparticle diffusion and Elovich kinetic models for the adsorption by N-coal, Z-coal, and PG, whereas the adsorption by raw coal is well fitted with both pseudo-second-order and Elovich kinetic models.
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    59. 59
      Faisal, M. L. F. M. Batch Sorption of Copper (II) Ions from Simulated Aqueous Solution by Banana Peel. Al-Khwarizmi Eng. J. 2017, 12 (4), 117– 125,  DOI: 10.22153/kej.2016.05.004
      There is no corresponding record for this reference.
    60. 60
      Mobarak, M.; Ali, R. A. M.; Seliem, M. K. Chitosan/Activated Coal Composite as an Effective Adsorbent for Mn(VII): Modeling and Interpretation of Physicochemical Parameters. Int. J. Biol. Macromol. 2021, 186, 750– 758,  DOI: 10.1016/j.ijbiomac.2021.07.089
      60
      Chitosan/activated coal composite as an effective adsorbent for Mn(VII): Modeling and interpretation of physicochemical parameters
      Mobarak, Mohamed; Ali, Rabea A. M.; Seliem, Moaaz K.
      International Journal of Biological Macromolecules (2021), 186 (), 750-758CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      Chitosan was impregnated into porous activated coal to produce a multifunctional chitosan/activated coal (Cs/Ac) composite. The resulted Cs/Ac was characterized and utilized as a cost-effective adsorbent for Mn(VII) at altered temps. (i.e., 25, 35, and 45°C). The adsorption results were fitted to classical as well as advanced statistical physics models. The Freundlich equation described well the achieved exptl. data at all temps. Enhancing the Langmuir adsorption capacity from 203.26 to 224.03 mg/g with temp. indicated that Mn(VII) adsorption was an endothermic process. Steric, energetic and thermodn. data of the double layer model with two energy sites (i.e., the best fit statistical model) were completely interpreted. The no. of Mn(VII) per adsorption site (n) was between 0.76 and 0.92 suggested the presence of multi-docking and multi-interactions mechanisms. The active sites d. (NM) of the Cs/Ac decreased with improving temp. Energetically, Mn(VII) uptake by Cs/Ac was governed by phys. interactions (i.e., adsorption energy <40 kJ/mol). Macroscopically, the interaction between Mn(VII) and Cs/Ac was spontaneous. Overall, modification of the Ac by the used marine biomass (Cs) produced a promising Mn(VII) adsorbent and also, the application of phys. anal. offered a deep interpretation for the adsorption mechanism.
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    61. 61
      Ashraf, M.-T.; AlHammadi, A. A.; El-Sherbeeny, A. M.; Alhammadi, S.; Al Zoubi, W.; Ko, Y. G.; Abukhadra, M. R. Synthesis of Cellulose Fibers/Zeolite-A Nanocomposite as an Environmental Adsorbent for Organic and Inorganic Selenium Ions; Characterization and Advanced Equilibrium Studies. J. Mol. Liq. 2022, 360, 119573  DOI: 10.1016/j.molliq.2022.119573
      61
      Synthesis of cellulose fibers/Zeolite-A nanocomposite as an environmental adsorbent for organic and inorganic selenium ions; Characterization and advanced equilibrium studies
      Ashraf, Menna-Tullah; AlHammadi, Ali A.; El-Sherbeeny, Ahmed M.; Alhammadi, Salh; Al Zoubi, Wail; Ko, Young Gun; Abukhadra, Mostafa R.
      Journal of Molecular Liquids (2022), 360 (), 119573CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
      Cellulose fibers/Zeolite-A composite (CF/ZA) was synthesized as an innovative hybrid structure of enhanced adsorption properties for different selenium species (inorg. (selenate (Se VI)), selenite (Se (IV)), and org. (selenomethionine (SeMt)). The CF/ZA composite achieved actual adsorption capacities of 163 mg/g (Se (VI)), 212.4 mg/g (Se (IV)), and 109.3 mg/g (SeMt) which are higher values than zeolite, cellulose, and several studied adsorbents in literature. The kinetic and classic equil. studies are in agreement with Pseudo-First order kinetics (R2 > 0.95) and Langmuir isotherm (R2 > 0.89). This suggests homogenous, monolayer, and more phys. uptake of the three selenium species. The monolayer model of one energy was assessed as an advanced equil. model. Based on the steric n parameter (2.88-3.31(Se (VI), 2.22-5.94 (Se (IV), and 3.46-4.41 (SeMt)) demonstrate the adsorption of them as three or more ions per each site in a vertical orientation by multi-ionic mechanisms. The adsorption energies (-20.78 to -27.14 kJ/mol) are related to physisorption processes such as hydrogen bonding (<30 kJ/mol) and dipole bonding forces (2-29 kJ/mol). The Gaussian energies (1.04-2.09 kJ/mol) support the physisorption reactions in addn. to zeolitic ion exchange processes. The thermodn. functions (internal energy, free enthalpy, and entropy) demonstrate the exothermic, feasible, and spontaneous properties of the reactions.
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    62. 62
      Dhaouadi, F.; Sellaoui, L.; Reynel-Ávila, H. E.; Landín-Sandoval, V.; Mendoza-Castillo, D. I.; Jaime-Leal, J. E.; Lima, E. C.; Bonilla-Petriciolet, A.; Lamine, A. B. Adsorption Mechanism of Zn2+, Ni2+, Cd2+, and Cu2+ Ions by Carbon-Based Adsorbents: Interpretation of the Adsorption Isotherms via Physical Modelling. Environmental Science and Pollution Research 2021, 28 (24), 30943– 30954,  DOI: 10.1007/s11356-021-12832-x
      62
      Adsorption mechanism of Zn2+, Ni2+, Cd2+, and Cu2+ ions by carbon-based adsorbents: interpretation of the adsorption isotherms via physical modelling
      Dhaouadi, Fatma; Sellaoui, Lotfi; Reynel-Avila, Hilda Elizabeth; Landin-Sandoval, Veronica; Mendoza-Castillo, Didilia I.; Jaime-Leal, Jose Enrique; Lima, Eder Claudio; Bonilla-Petriciolet, Adrian; Lamine, Abdelmottaleb Ben
      Environmental Science and Pollution Research (2021), 28 (24), 30943-30954CODEN: ESPLEC; ISSN:0944-1344. (Springer)
      A theor. physicochem. and thermodn. investigation of the adsorption of heavy metals Zn2+, Cd2+, Ni2+, and Cu2+ on carbon-based adsorbents was performed with statistical physics fundaments. Particularly, the exptl. adsorption isotherms of heavy metal removal, at 30°C and pH 5, using adsorbents obtained from the pyrolysis of three biomasses (cauliflower cores, broccoli stalks, and coconut shell) were modelled and interpreted with a homogeneous statistical physics adsorption model. Calcns. indicated that the heavy metal adsorption with these carbon-based materials was a multi-ionic process where several ions interact simultaneously with the same carboxylic functional group on the adsorbent surface. Adsorption capacities for these metal ions and adsorbents were correlated with electronegativity theory, which established that the adsorbate with the highest electronegativity was more readily adsorbed by the carboxylic functional groups available on the adsorbent surfaces. Also, the chem. compns. of biomass precursors explained achieved adsorption capacities for these metallic ions. The best adsorbent for heavy metal removal was obtained from CC biomass pyrolysis. Calcd. adsorption energies for heavy metal removal could be assocd. with physisorption-type forces. Finally, the adsorption mechanism anal. was complemented with the detn. of adsorption thermodn. functions using the statistical physics.
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    63. 63
      Sellaoui, L.; Ali, J.; Badawi, M.; Bonilla-Petriciolet, A.; Chen, Z. Understanding the Adsorption Mechanism of Ag+ and Hg2+ on Functionalized Layered Double Hydroxide via Statistical Physics Modeling. Appl. Clay Sci. 2020, 198, 105828  DOI: 10.1016/j.clay.2020.105828
      63
      Understanding the adsorption mechanism of Ag+ and Hg2+ on functionalized layered double hydroxide via statistical physics modeling
      Sellaoui, Lotfi; Ali, Jawad; Badawi, Michael; Bonilla-Petriciolet, Adrian; Chen, Zhuqi
      Applied Clay Science (2020), 198 (), 105828CODEN: ACLSER; ISSN:0169-1317. (Elsevier B.V.)
      Modeling anal. based on a statistical physics theory was used to explain the adsorption of Ag+ and Hg2+ on layered double hydroxides (LDH) functionalized with anions CO32-, NO3-, S52- and MoS42-. Theor. adsorption models assuming different types of functional groups on LDH surface were tested and compared. A statistical physics model based on two active sites for the adsorbate binding was the best option to characterize and interpret the removal of investigated heavy metals on LDH. Modeling results showed that the total adsorption capacities at satn. ranged from 112 to 631 mg/g and from 110 to 638 mg/g for Ag+ and Hg2+, resp. LDH functionalized with anion MoS2-4 was the best adsorbent for the removal of both metal ions. It was also demonstrated that the anionic functionalities and the oxygen-contg. groups of LDH contributed in different extent for the adsorption of Ag+ and Hg2+. Statistical physics parameters suggested a multi-ionic and endothermic adsorption caused by phys. and chem. interactions. Finally, the adsorption mechanism was macroscopically explained via the calcn. and anal. of thermodn. potentials.
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    64. 64
      Ali, R. A. M.; Mobarak, M.; Badawy, A. M.; Lima, E. C.; Seliem, M. K.; Ramadan, H. S. New Insights into the Surface Oxidation Role in Enhancing Congo Red Dye Uptake by Egyptian Ilmenite Ore: Experiments and Physicochemical Interpretations. Surfaces and Interfaces 2021, 26, 101316  DOI: 10.1016/j.surfin.2021.101316
      64
      New insights into the surface oxidation role in enhancing Congo red dye uptake by Egyptian ilmenite ore: Experiments and physicochemical interpretations
      Ali, Rabea A. M.; Mobarak, Mohamed; Badawy, Aliaa M.; Lima, Eder C.; Seliem, Moaaz K.; Ramadan, H. S.
      Surfaces and Interfaces (2021), 26 (), 101316CODEN: SIUNCN; ISSN:2468-0230. (Elsevier B.V.)
      The continuous discharge of org. dyes into the aquatic environment represents a main reason for water contamination. Removal of dye mols. via adsorption is suggested to be an effective, simple, and low-cost technol. Herein, two representative samples of black ilmenite and its oxidized red form were characterized and tested as adsorbents for Congo red (CR) dye. The high concns. of iron-titanium oxides in the red ilmenite was due to the surface alteration. The red ilmenite displayed high adsorption capacities against CR compared to the black one at varied pH values (i.e. 5.0-9.0). The Freundlich model described well the CR data at all adsorption temps. (25, 40, and 50°C). The physicochem. parameters of the multilayer model were employed to recognize the interface mechanisms between CR mols. and the ilmenite active sites. The values of receptor sites (n) ranged from 0.60 to 0.91 (i.e., n < 1.0 at all temps.) suggesting a horizontal position and multi-docking adsorption mechanism. In the temp. range of 25-50°C, the increase of the total removed CR layers (the Nt parameter) from 2.9 to 4.4 resulted in enhancing the adsorption capacity at satn. (Qsat) from 158.23 to 267.96 mg/g. The values of adsorption energies varied from 13.26 to 18.356 kJ/mol reflected that CR adsorption onto the RI was endothermic and assocd. to phys. interactions. Overall, the high performance of the red ilmenite was mainly assocd. with the control of surface alteration. Furthermore, utilizing the multilayer statistical model described the interaction mechanism between CR and ilmenite adsorption sites at mol. level.
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    65. 65
      Dhaouadi, F.; Sellaoui, L.; Badawi, M.; Reynel-Ávila, H. E.; Mendoza-Castillo, D. I.; Jaime-Leal, J. E.; Bonilla-Petriciolet, A.; Lamine, A. B. Statistical Physics Interpretation of the Adsorption Mechanism of Pb2+, Cd2+ and Ni2+ on Chicken Feathers. J. Mol. Liq. 2020, 319, 114168  DOI: 10.1016/j.molliq.2020.114168
      65
      Statistical physics interpretation of the adsorption mechanism of Pb2+, Cd2+ and Ni2+ on chicken feathers
      Dhaouadi, Fatma; Sellaoui, Lotfi; Badawi, Michael; Reynel-Avila, Hilda Elizabeth; Mendoza-Castillo, Didilia Ileana; Jaime-Leal, Jose Enrique; Bonilla-Petriciolet, Adrian; Lamine, Abdelmottaleb Ben
      Journal of Molecular Liquids (2020), 319 (), 114168CODEN: JMLIDT; ISSN:0167-7322. (Elsevier B.V.)
      The mechanism of adsorption of Pb2+, Cd2+ and Ni2+ on chicken feathers was studied via statistical physics theory. A detailed theor. anal. was performed using three models that assumed the adsorption of these metal ions via one, two or three types of surface functionalities from chicken feathers. These surface functionalities corresponded to carboxylic, disulfide and amino groups. The monolayer adsorption model with two types of functional groups was selected to analyze the steric and energetic factors involved in the removal of these heavy metals. Results of the statistical physics modeling showed that this adsorption system was multi-ionic with the presence of both endothermic and exothermic adsorption stages depending on soln. temp. Calcd. adsorption energies were assocd. to phys. adsorption forces where the carboxylic and disulfide functional groups were responsible of metal binding on chicken feathers. Thermodn. calcns. of configuration entropy, free enthalpy and internal energy indicated that the adsorption of Pb2+, Cd2+ and Ni2+ on chicken feathers was a spontaneous and feasible process. These findings contribute to understand and characterize the thermodn. nature of the adsorption of heavy metal ions on natural adsorbents like chicken feathers.
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    66. 66
      Shemy, M. H.; Othman, S. I.; Alfassam, H. E.; Al-Waili, M. A.; Alqhtani, H. A.; Allam, A. A.; Abukhadra, M. R. Synthesis of Green Magnetite/Carbonized Coffee Composite from Natural Pyrite for Effective Decontamination of Congo Red Dye: Steric, Synergetic, Oxidation, and Ecotoxicity Studies. Catalysts 2023, 13 (2), 264,  DOI: 10.3390/catal13020264
      66
      Synthesis of Green Magnetite/Carbonized Coffee Composite from Natural Pyrite for Effective Decontamination of Congo Red Dye: Steric, Synergetic, Oxidation, and Ecotoxicity Studies
      Shemy, Marwa H.; Othman, Sarah I.; Alfassam, Haifa E.; Al-Waili, Maha A.; Alqhtani, Haifa A.; Allam, Ahmed A.; Abukhadra, Mostafa R.
      Catalysts (2023), 13 (2), 264CODEN: CATACJ; ISSN:2073-4344. (MDPI AG)
      Green magnetite/carbonized spent coffee (MG/CFC) composite was synthesized from natural pyrite and characterized as an adsorbent and catalyst in photo-Fenton's oxidn. system of Congo red dye (C.R). The absorption behavior was illustrated based on the steric and energetic parameters of the advanced Monolayer equil. model of one energetic site (R2 > 0.99). The structure exhibits 855 mg/g as effective site d. which induces its C.R satn. adsorption capacity to 436.1 mg/g. The change in the no. of absorbed C.R per site with temp. (n = 1.53 (293) to 0.51 (313 K)) suggests changes in the mechanism from multimol. (up to 2 mols. per site) to multianchorage (one mol. per more than one site) processes. The energetic studies (ΔE = 6.2-8.2 kJ/mol) validate the phys. uptake of C.R by MG/CFC which might be included van der Waals forces, electrostatic attractions, and hydrogen bonding. As a catalyst, MG/CFC exhibits significant activity during the photo-Fenton's oxidn. of C.R under visible light. The complete oxidn. of C.R was detected after 105 min (5 mg/L), 120 min (10 mg/L), 135 min (15 mg/L), 180 min (20 mg/L), and 240 min (25 mg/L) using MG/CFC at 0.2 g/L dosage and 0.1 mL of H2O2. Increasing the dosage up to 0.5 g/L reduce the complete oxidn. interval of C.R (5 mg/L) down to 30 min while the complete mineralization was detected after 120 min. The acute and chronic toxicities of the treated samples demonstrate significant safe products of no toxic effects on aquatic organisms as compared to the parent C.R soln.
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    67. 67
      Sellaoui, L.; Guedidi, H.; SarraWjihi, S.; Reinert, L.; Knani, S.; Duclaux, L.; Ben Lamine, A. Experimental and Theoretical Studies of Adsorption of Ibuprofen on Raw and Two Chemically Modified Activated Carbons: New Physicochemical Interpretations. RSC Adv. 2016, 6 (15), 12363– 12373,  DOI: 10.1039/C5RA22302D
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      Experimental and theoretical studies of adsorption of ibuprofen on raw and two chemically modified activated carbons: new physicochemical interpretations
      Sellaoui, Lotfi; Guedidi, Hanen; SarraWjihi; Reinert, Laurence; Knani, Salah; Duclaux, Laurent; Ben Lamine, Abdelmottaleb
      RSC Advances (2016), 6 (15), 12363-12373CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
      Knowledge of the ibuprofen (IBP) adsorption isotherms is important to understand and to improve its depollution process. In this work, the double layer model with two energies was applied to simulate the adsorption isotherms of ibuprofen on raw activated and two chem. modified granular activated carbons, obtained exptl. at pH = 7 and at different temps. (298, 313 and 323 K). The chem. modified samples were obtained by treatment at 700°C under nitrogen flow and ultrasonic treatment in H2O2 soln. of the raw granulated activated carbon. The establishment of the model is based on a statistical physics approach, particularly on the grand canonical ensemble. The double layer model with two energies for each layer was found to be the best model to describe the adsorption process of ibuprofen. Using this model, the different adsorption isotherms of ibuprofen were described sterically and energetically through these parameters. The different parameters were interpreted as a function of temp. In addn. to this, the entropy, free enthalpy and the internal energy governing the adsorption process were calcd. and interpreted.
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    68. 68
      Zafar, M. N.; Amjad, M.; Tabassum, M.; Ahmad, I.; Zubair, M. SrFe2O4 Nanoferrites and SrFe2O4/Ground Eggshell Nanocomposites: Fast and Efficient Adsorbents for Dyes Removal. Journal of Cleaner Production 2018, 199, 983– 994,  DOI: 10.1016/j.jclepro.2018.07.204
      68
      SrFe2O4 nanoferrites and SrFe2O4/ground eggshell nanocomposites: Fast and efficient adsorbents for dyes removal
      Zafar, Muhammad Nadeem; Amjad, Mufarah; Tabassum, Mehwish; Ahmad, Iqbal; Zubair, Muhammad
      Journal of Cleaner Production (2018), 199 (), 983-994CODEN: JCROE8; ISSN:0959-6526. (Elsevier Ltd.)
      In recent years nanomaterials are attracting much attention in water pollution treatment due to their greater surface area and unique properties. In this work, a micro emulsion method had been successfully utilized to synthesize novel strontium nanoferrites, SrFe2O4 an efficient adsorbent for both anionic dye erichrome black T and cationic dye methylene blue. To further improve the efficiency of SF, eggshells powder was employed as a support or co sorbent to produce another adsorbent named SF@EgP by combining EgP and SF using solvothermal method. The adsorbents were characterized by XRD, SEM techniques and further impendence spectroscopy and electrochem. characterization was also performed for SF. The SF and SF@EgP were tuned for EBT and MB removal and proved to be novel and efficient adsorbents and their adsorption efficiency was also compared with EgP. Using these model dyes, we investigated the influence of pH, adsorbent quantity, time and initial dyes concns. on adsorption. The adsorption process of EBT and MB was examd. by kinetics, isothermal and thermodn. modeling that resp. directed that the removal of dyes was much quicker. In addn., the SF and SF@EgP were regenerated and recycled successfully showing their reusability. In short these novel adsorbents not only tunable and showed reusability for cationic and anionic dyes with fast adsorption but also provide valuable clues towards synthesis and adsorption studies of other nanomaterials.
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    69. 69
      Yildirim, A.; Bulut, Y. Adsorption Behaviors of Malachite Green by Using Crosslinked Chitosan/Polyacrylic Acid/Bentonite Composites with Different Ratios. Environmental Technology & Innovation 2020, 17, 100560  DOI: 10.1016/j.eti.2019.100560
      69
      Adsorption behaviors of malachite green by using crosslinked chitosan/polyacrylic acid/bentonite composites with different ratios
      Yildirim, Ayfer; Bulut, Yasemin
      Environmental Technology & Innovation (2020), 17 (), 100560CODEN: ETINBL; ISSN:2352-1864. (Elsevier B.V.)
      In this study, by using different quantities of methylenebisacrylamide (MBA) and acrylic acid (AA), chitosan/polyacrylic acid/bentonite composites (CCS/PAA/BNTs) were synthesized and used for the adsorption of malachite green (MG). The fourier transmission IR spectra, thermogravimetric anal.-DTA and SEM techniques were used to det. synthesized composites. The effects of initial concn., contact time, temp. and pH were investigated. Kinetic studies indicated that, due to the pseudo-second order model, correlation coeffs. (R2>0.98) were the best fit thus, by using kps, the activation energies (Ea) were calcd.(19.06, 15.64, 19.49, 8.29, 24.53 kJmol-1). The equil. data of MG agreed with the Langmuir model. The highest adsorption capacity calcd. was found as 384.62-454.55 mgg-1 for MG adsorption at 298-318 K. Thermodn. studies demonstrated that MG adsorption was endothermic, caused spontaneous reaction and increased the entropy between 298-318 K. The adsorption reactions of MG were revealed as physisorption (ΔH<80 kjmol-1). The optimum pH was found as 6. The CCS/PAA/BNT2 composite indicated the highest adsorption capacity and best thermal stability compared to the other composites.
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    70. 70
      Jiang, M.; Chen, L.; Niu, N. Enhanced Adsorption for Malachite Green by Functionalized Lignin Magnetic Composites: Optimization, Performance and Adsorption Mechanism. J. Mol. Struct. 2022, 1260, 132842  DOI: 10.1016/j.molstruc.2022.132842
      70
      Enhanced adsorption for malachite green by functionalized lignin magnetic composites: Optimization, performance and adsorption mechanism
      Jiang, Minwen; Chen, Ligang; Niu, Na
      Journal of Molecular Structure (2022), 1260 (), 132842CODEN: JMOSB4; ISSN:0022-2860. (Elsevier B.V.)
      Herein, a novel kind of magnetic amino-modified lignin (MAL) sorbents was designed through a facile strategy based on Mannich reaction, which was used for removing a typical aquatic pollutant malachite green (MG). During the synthesis procedure, the 3-amino-propyltriethoxysilane was used as the cross-linker between aminated lignin and magnetic nanoparticles. The phys. and chem. structure of MAL were investigated through a series of characterization methods including FTIR, XRD, TGA, SEM, and XPS. The effect of pH shows that the adsorbent has excellent adsorption performance for MG at pH=7. According to the adsorption data, the adsorption process was in line with the Langmuir model and the pseudo-second-order model, indicating that the adsorption was monolayer adsorption and chemisorption. MAL showed excellent sorption capacity of 456.62 mg/g and high adsorption speed within 35 min. Thermodn. studies show that the adsorption is exothermic and spontaneous. Meanwhile, MAL shows good magnetic properties with the satn. magnetization intensities of 22.61 emu/g. In addn., the MAL could be easily recovered and reused at least five times, which performed good reusability. The mechanism of MG capture onto MAL can be mainly attributed to electrostatic attraction, hydrogen bonding, and π-π stacking. In a word, the as-prepd. MAL showed great potential for wastewater treatment due to its excellent adsorption efficiency, environmental friendliness, and superparamagnetic behavior.
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    71. 71
      Gupta, K.; Khatri, O. P. Reduced Graphene Oxide as an Effective Adsorbent for Removal of Malachite Green Dye: Plausible Adsorption Pathways. J. Colloid Interface Sci. 2017, 501, 11– 21,  DOI: 10.1016/j.jcis.2017.04.035
      71
      Reduced graphene oxide as an effective adsorbent for removal of malachite green dye: Plausible adsorption pathways
      Gupta, Kanika; Khatri, Om P.
      Journal of Colloid and Interface Science (2017), 501 (), 11-21CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)
      Efficient removal of malachite green (MG) dye from simulated wastewater is demonstrated using high surface area reduced graphene oxide (rGO). The plausible interaction pathways between MG dye and rGO are deduced from nanostructural features (HRTEM) of rGO and spectroscopic analyses (FTIR and Raman). The high surface area (931 m2 gm-1) of rGO, π-π interaction between the arom. rings of MG dye and graphitic skeleton, and electrostatic interaction of cationic center of MG dye with π-electron clouds and neg. charged residual O functionalities of rGO collectively facilitate the adsorption of MG dye on the rGO. The rGO displays adsorption capacity ≤476.2 mg g-1 for MG dye. The thermodn. parameters calcd. from the temp. dependent isotherms suggested that the adsorption was a spontaneous and endothermic process. These results promise the potential of high surface area rGO for efficient removal of cationic dyes for wastewater treatment.
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    72. 72
      Sricharoen, P.; Kongsri, S.; Kukusamude, C.; Areerob, Y.; Nuengmatcha, P.; Chanthai, S.; Limchoowong, N. Ultrasound-Irradiated Synthesis of 3-Mercaptopropyl Trimethoxysilane-Modified Hydroxyapatite Derived from Fish-Scale Residues Followed by Ultrasound-Assisted Organic Dyes Removal. Sci. Rep. 2021, 11 (1), 5560,  DOI: 10.1038/s41598-021-85206-5
      72
      Ultrasound-irradiated synthesis of 3-mercaptopropyl trimethoxysilane-modified hydroxyapatite derived from fish-scale residues followed by ultrasound-assisted organic dyes removal
      Sricharoen, Phitchan; Kongsri, Supalak; Kukusamude, Chunyapuk; Areerob, Yonrapach; Nuengmatcha, Prawit; Chanthai, Saksit; Limchoowong, Nunticha
      Scientific Reports (2021), 11 (1), 5560CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)
      We report a novel method for the synthesis of 3-mercaptopropyl trimethoxysilane-modified hydroxyapatite (FHAP-SH) derived from fish-scale residues by using ultrasound irradn. SEM, transmission electron microscopy, energy-dispersive spectroscopy, X-ray diffraction, and Fourier transform IR spectroscopy were used for the FHAP-SH characterization. Then, the org. dye adsorption on the FHAP-SH was monitored through an ultrasound process. After the dye removal optimization, significant improvements were obsd. in the max. adsorption capacities for Congo Red (CR, 500 mg g-1), Coomassie Brilliant Blue G 250 (CB, 235 mg g-1), and Malachite Green (MG, 625 mg g-1). The adsorption behaviors of these dyes were fitted by using the Langmuir isotherm model with a high coeff. of detn. values ranging from 0.9985 to 0.9969. The adsorption of the three dyes onto FHAP-SH was an endothermic process based on the adsorption thermodn. model, while the adsorption kinetics anal. of the dyes presented a good alignment with the pseudo-second-order kinetics. The FHAP-SH exhibits a remarkably high adsorption capacity, is inexpensive, and fulfills the ecofriendly requirements of dye wastewater treatment, esp. in the textile industry.
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    73. 73
      Zaidi, N. A. H. M.; Lim, L. B. L.; Usman, A. Enhancing Adsorption of Malachite Green Dye Using Base-Modified Artocarpus Odoratissimus Leaves as Adsorbents. Environmental Technology & Innovation 2019, 13, 211– 223,  DOI: 10.1016/j.eti.2018.12.002
      There is no corresponding record for this reference.
    74. 74
      Gao, M.; Wang, Z.; Yang, C.; Ning, J.; Zhou, Z.; Li, G. Novel Magnetic Graphene Oxide Decorated with Persimmon Tannins for Efficient Adsorption of Malachite Green from Aqueous Solutions. Colloids Surf., A 2019, 566, 48– 57,  DOI: 10.1016/j.colsurfa.2019.01.016
      74
      Novel magnetic graphene oxide decorated with persimmon tannins for efficient adsorption of malachite green from aqueous solutions
      Gao, Mingmin; Wang, Zhongmin; Yang, Chengxian; Ning, Jinliang; Zhou, Zhide; Li, Guiyin
      Colloids and Surfaces, A: Physicochemical and Engineering Aspects (2019), 566 (), 48-57CODEN: CPEAEH; ISSN:0927-7757. (Elsevier B.V.)
      Dyeing effluent is one of the main sources of textile wastewater, which has a seriously destructive impact on human health. A simple and effective way to remove dyes from the environment is required. In this paper, a new adsorbent, magnetic graphene oxide decorated with persimmon tannins (Fe3O4/PT/GO) composites, has been prepd. by one-step hydrothermal method for efficient adsorption of malachite green (MG) from aq. solns. The microstructure and compn. of the Fe3O4/PT/GO adsorbent were characterized by SEM, Fourier transform IR (FTIR) spectroscopy, Brunauer-Emmett-Teller (BET) anal., X-ray powder diffraction (XRD) and vibrating sample magnetometer (VSM). The Fe3O4/PT/GO adsorbent had excellent adsorption ability with the max. adsorption capacity of 560.58 mg/g at 308 K and pH 6.0. The adsorption capacity maintained 85.9% after five cycles. The adsorption process of MG conformed to the Langmuir isotherm model and pseudo-second order kinetic equations. In addn., the thermodn. studies indicated that the adsorption process is spontaneous and endothermic. All the exptl. results showed that the Fe3O4/PT/GO adsorbent had good adsorption capacity for removing MG from wastewater and can be quickly extd. from water under an external magnetic field.
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    75. 75
      Raval, N. P.; Shah, P. U.; Shah, N. K. Malachite Green “a Cationic Dye” and Its Removal from Aqueous Solution by Adsorption. Applied Water Science 2017, 7 (7), 3407– 3445,  DOI: 10.1007/s13201-016-0512-2
      75
      Malachite green "a cationic dye" and its removal from aqueous solution by adsorption
      Raval, Nirav P.; Shah, Prapti U.; Shah, Nisha K.
      Applied Water Science (2017), 7 (7), 3407-3445CODEN: AWSPCL; ISSN:2190-5495. (Springer GmbH)
      Adsorption can be efficiently employed for the removal of various toxic dyes from water and wastewater. In this article, the authors reviewed variety of adsorbents used by various researchers for the removal of malachite green (MG) dye from an aq. environment. The main motto of this review article was to assemble the scattered available information of adsorbents used for the removal of MG to enlighten their wide potential. In addn. to this, various optimal exptl. conditions (soln. pH, equil. contact time, amt. of adsorbent and temp.) as well as adsorption isotherms, kinetics and thermodn. data of different adsorbents towards MG were also analyzed and tabulated. Finally, it was concluded that the agricultural solid wastes and biosorbents such as biopolymers and biomass adsorbents have demonstrated outstanding adsorption capabilities for removal of MG dye.
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  • Supporting Information

    Supporting Information

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsomega.3c07870.

    • Representative equations of the kinetic and isotherm models (Table S1) (PDF)


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