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Bacterial Cellulose Aerogels Derived from Pineapple Peel Waste for the Adsorption of Dyes
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  • Ha Vu Le
    Ha Vu Le
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    More by Ha Vu Le
  • Nghia Thi Dao
    Nghia Thi Dao
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    More by Nghia Thi Dao
  • Ha Truc Bui
    Ha Truc Bui
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    More by Ha Truc Bui
  • Phung Thi Kim Le
    Phung Thi Kim Le
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    More by Phung Thi Kim Le
    Orcidhttps://orcid.org/0000-0003-0570-3154
  • Kien Anh Le
    Kien Anh Le
    Institute for Tropical Technology and Environmental Protection, 57A Truong Quoc Dung, Phu Nhuan District, Ho Chi Minh City 726500, Viet Nam
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  • An Thi Tuong Tran
    An Thi Tuong Tran
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    More by An Thi Tuong Tran
  • Khoa Dang Nguyen*
    Khoa Dang Nguyen
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    *Email: [email protected]
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  • Hanh Huynh Mai Nguyen*
    Hanh Huynh Mai Nguyen
    Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam
    Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    *Email: [email protected]
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  • Phuoc Hoang Ho*
    Phuoc Hoang Ho
    Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg SE-412 96, Sweden
    *Email: [email protected]
    More by Phuoc Hoang Ho
    Orcidhttps://orcid.org/0000-0001-8571-4114
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ACS Omega

Cite this: ACS Omega 2023, 8, 37, 33412–33425
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https://doi.org/10.1021/acsomega.3c03130
Published September 1, 2023

Copyright © 2023 The Authors. Published by American Chemical Society. This publication is licensed under

CC-BY 4.0 .

Abstract

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Valorization of pineapple peel waste is an attractive research topic because of the huge quantities of this byproduct generated from pineapple processing industries. In this study, the extract from pineapple waste was collected to produce a hydrogel-like form containing bacterial cellulose fibers with a three-dimensional structure and nanoscale diameter by the Acetobacter xylinum fermentation process. The bacterial cellulose suspension was subsequently activated by freeze-drying, affording lightweight aerogels as potential adsorbents in wastewater treatment, in particular the adsorptive removal of organic dyes. Intensive tests were carried out with the adsorption of methylene blue, a typical cationic dye, to investigate the influence of adsorption conditions (temperature, pH, initial dye concentration, time, and experiment scale) and aerogel-preparation parameters (grinding time and bacterial cellulose concentration). The bacterial cellulose-based aerogels exhibited high adsorption capacity not only for methylene blue but also for other cationic dyes, including malachite green, rhodamine B, and crystal violet (28–49 mg/g). However, its activity was limited for most of the anionic dyes, such as methyl orange, sunset yellow, and quinoline yellow, due to the repulsion of these anionic dyes with the aerogel surface, except for the case of congo red. It is also an anionic dye but has two amine groups providing a strong interaction with the hydroxyl group of the aerogel via hydrogen bonding. Indeed, the aerogel has a substantially large congo red-trapping capacity of 101 mg/g. Notably, the adsorption process exhibited similar performances, upscaling the solution volume to 50 times. The utilization of abundant agricultural waste in the simple aerogel preparation to produce a highly efficient and biodegradable adsorbent is the highlight of this work.

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1. Introduction

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Water plays a vital role in human life and human activities. (1,2) However, explosive development in the manufacture of textiles, paints, leather, pharmaceuticals, and personal care products has resulted in the release of numerous organic toxins such as dyes, solvents, surfactants, and organometallic substances into the aqueous medium. (3−6) Due to the carcinogenic, mutagenic, and allergenic effects of dyes and their increasing presence in various water resources, it is indeed necessary to thoroughly remove these toxic compounds from wastewater. (7) Various methods have been suggested for the treatment of dye wastewater, including oxidation, coagulation, adsorption, irradiation, ion exchange, membrane separation, and biological processes. (8) Among them, the adsorption method is favored because of its simplicity, high efficiency, and low cost. (9−12) The discovery of efficient adsorbents plays an important role in adsorption technology. Moreover, from a sustainable development point of view, finding new environment-friendly porous biomaterials for capturing organic dyes from aqueous solutions is highly encouraged. (13)
Recently, aerogels have become known as a typical class of three-dimensional (3D) materials with a high degree of porosity and desirable properties for various applications, for example, air cleaning, water treatment, catalysis, or energy storage. (14,15) These materials could be produced from various components such as silica, carbon, metal oxides, or organic polymers. However, the frameworks derived from polysaccharides, including cellulose, starch, chitosan, alginate, and pectin, have specifically drawn much attention because of their renewability as well as abundance in nature. (16) Among these resources, bacterial cellulose (BC) exhibits interesting chemical and physical properties, including high crystallinity (>80%), a disordered 3D framework, good tensile strength, and moldability due to the formation of uniform nanofibers during the fermentation of carbohydrates by A. xylinum. (17,18) Especially, in comparison with the utilization of plant cellulose, one of the most important benefits provided by bacterial cellulose is the absence of lignin and hemicellulose, which were removed under complicated and harsh conditions using hazardous chemicals. (19−21) On the other hand, carbohydrate-containing agricultural commodities, e.g., coconut water and fruit extracts, have been widely used to fermentatively produce high-purity and low-cost cellulose on commercial scales for well-known applications in food and pharmaceuticals. (22−28) Based on such outstanding features, bacterial cellulose is considered as a promising renewable material for yielding functional aerogels toward removing harmful contaminants such as organic dyes and heavy-metal cations from aqueous solutions. (18)
In this work, pineapple peel waste collected from pineapple-based food manufacturing processes was employed as an abundant carbohydrate source to produce bacterial cellulose via fermentation at ambient conditions. The bacterial cellulose was subsequently transformed into lightweight aerogels using a freeze-drying method. The characterizations of BC-based aerogels were performed by different techniques, including powder X-ray diffraction (PXRD), thermogravimetric analysis (TGA), nitrogen physisorption at 77 K, and scanning electron microscopy (SEM), to confirm the non-ordered and porous 3D structure of the bacterial cellulose network in the aerogels. These biomaterials were applied as green and inexpensive adsorbents for the removal of organic dyes from water, showing promising performances without any further chemical modification.

2. Material and Methods

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All chemicals were purchased from Sigma-Aldrich and Acros and used as received without any further purification.

2.1. Synthesis of Aerogel

The extract of pineapple peel waste (Ananas comosus Spanish, planted in Long An, Viet Nam) was collected, filtrated, and fermented by A. xylinum under aerobic conditions. (29) After 7 days, a hydrogel-like layer with a thickness of approx. 2 cm formed on the surface of the fermentative phase, which is commonly known as nata de pina, was collected. Raw nata de pina (Figure 1a) was immersed in a sodium hydroxide solution (1 M) for 12 h and subsequently washed with water until neutralization (Figure 1b).

Figure 1

Figure 1. Photographs of (a) 100-g batch of the nata de pina preparation via the fermentation of the extract of pineapple peel waste and (b) nata de pina after washing with NaOH and water, sequentially.

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Prior to further experiments, the washed nata de pina samples were cut into approx. one-centimeter cubes. The cellulose content was determined to be approx. 0.80 wt % based on drying the washed sample at 120 °C for 24 h. Nata de pina pieces were mixed with water in a 1:1 ratio. The mixture was subsequently ground using a Philips HR2531 hand blender at 650 W for different time intervals (1–5 min) and added with water to obtain a suspension with a predetermined BC content (0.24 to 0.80 wt %). The obtained mixtures were then subsequently frozen at −20 °C for 24 h. The bacterial cellulose aerogels were obtained by freeze-drying the frozen samples at 0.5 mbar for 48 h using a Toption TPV-50F vacuum freeze dryer to produce cylinder-shaped aerogel samples with a typical diameter of approx. 6.5 cm (d) and thickness of approx. 3.0 cm (h).
Bulk density of the collected aerogel samples was determined via the equation ρa =4·m/π × d2 × h in which m, d, and h are, respectively, the weight, diameter, and thickness of the samples.
Porosity of aerogel samples was calculated via the equation Ø = 100 × (1 – ρa/ρb) in which ρa is the bulk of cellulose aerogels (g/cm3) and ρb is the crystalline cellulose density (1.5 g/cm3). (30−32)

2.2. Adsorption Study

Adsorption capacity of aerogel was investigated for two groups of organic dyes, including cationic dyes (methylene blue, rhodamine B, crystal violet, and malachite green) and anionic dyes (methyl orange, quinoline yellow, sunset yellow, and congo red) (Table 1). In a typical experiment, approx. 20 mg of the BC aerogel was loaded into 10 mL of a solution containing 50 ppm of methylene blue (MB). The adsorption was performed at 30 °C under vigorous stirring for 30 min. The aerogel was subsequently separated from the solution by filtration. The MB concentrations in the solution before and after the adsorption course were determined by ultraviolet–visible (UV–vis) spectroscopy using a G10S UV–vis device (Thermo Scientific, Waltham, Massachusetts, USA). Additionally, the experiments for the MB adsorption and the aerogel preparation were also performed at different conditions to study the effect of temperature (20–60 °C), pH (3.6–11.0), initial dye concentration (0–400 ppm), adsorption time (0–120 min), bacterial cellulose content (0.24–0.80 wt.%), grinding time (1–5 min), and experiment scale (10–500 mL) on the MB trapping efficiency. The error bar for each data point was the standard deviation from three experiments.
Table 1. Details of Organic Dyes Used in This Study
*

Sizes of the organic dye molecules (length x width) were estimated by the Materials Studio program.

Two models including pseudo-first-order and pseudo-second-order equations (eqs 1 and 2) were applied to study the kinetics of the MB adsorption by the BC aerogel. (33)
ln(Qe−Qt)=ln⁡Qe−k1×t
(1)
tQt=tk2×1Qt2+1Qet
(2)
in which Qe is the adsorption capacity at the equilibrium (mg/g), Qt is the adsorption capacity at a given time (mg/g), k1 and k2 are the rate constants of the adsorption models, respectively. (33)
The interaction of the MB molecules with the BC surface was also investigated by employing the Langmuir and Freundlich adsorption isotherm equations (eqs 3 and 4). (34)
CeQe=1KL×Q+CeQo
(3)
ln⁡Qe=1nln⁡Ce+ln⁡KF
(4)
in which Qe is the adsorption capacity at the equilibrium (mg/g), Ce is the equilibrium concentration in solution (mg/L, ppm), Qo is the maximum amount of adsorption (mg/g), and KL and KF are the Langmuir and Freundlich constants, respectively. (34)
For the recycling test, the aerogel was collected from a 500 mL-scale experiment by gravity filtration before being washed with acetone containing 5 wt % of HCl five times to remove MB. The resulting bacterial cellulose phase was subsequently washed with water until neutralization. This washed bacterial cellulose suspension was frozen at −20 °C for 24 h and freeze-dried, yielding the regenerated aerogel for the next adsorption experiment under identical conditions.

2.3. Material Characterization

Textural properties of the cellulose materials were determined by nitrogen physisorption at 77 K using an ASAP 2020 instrument (Micromeritics, USA). Before each analysis, samples were degassed at 60 °C under vacuum for 12 h. The specific surface area was determined over a relative pressure range of P/Po = 0.05–0.30 using the Brunauer–Emmett–Teller (BET) method.
PXRD patterns were obtained on a D8 ADVANCE diffractometer (Bruker AXS, Germany) using Ni-filtered Cu Kα radiation. Each measurement was performed in a 2θ range of 10–70° with an angular step size of 0.0105° and a scanning rate of 0.63° per min.
Morphology of the aerogel samples was recorded by field-emission SEM (FESEM) using a Hitachi S-4800 microscope with a magnification of 25,000× at an accelerating voltage of 10 kV.
Thermal stability of cellulose was analyzed by TGA on a TA Instruments SDT Q600 thermal gravimetric analyzer. Approx. 10 mg of the aerogel sample was placed into an alumina pan, and the sample was heated from 30 to 900 °C at a rate of 10 °C/min in air.
Average size of the nata de pina suspension mixture after grinding was determined by laser diffraction spectroscopy using a Horiba LA-950V2 laser diffraction spectrometry.
Fourier transform infrared spectroscopy (FT-IR) measurement was performed using a Bruker Vertex 70 spectrometer for the aerogel sample dispersed on a potassium bromide pellet. Each measurement was accumulated from 32 scans at a resolution of 4 cm–1 recorded in the 4000–500 cm–1 range.
The point of zero charge (pHPZC) of the BC aerogel material derived was determined by monitoring the pH change of a 1.0 mol/L NaCl solution with varied pH. (35) In detail, the pH value (pH1) of the initial NaCl solution was predetermined in the range of 3–11 by adding a 5 wt % solution of HCl or NaOH. 20 mg of the aerogel was subsequently added to the obtained NaCl solution. After 24 h under vigorous stirring, the solution pH (pH2) was measured again. The pH difference (ΔpH = pH2–pH2) was plotted versus pH1, and pHPZC was the vertical projection of the curve.

3. Results and Discussion

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3.1. Material Characterization

In this study, nata de pina containing approx. 0.80 wt % of bacterial cellulose was produced from the pineapple peel extract for many different batches (approx. 100 g of nata de pina per batch) without the addition of any further nutrients and carbohydrate resources. The PXRD pattern of the BC aerogel material prepared from the nata de pina hydrogel showed featured reflections of crystalline cellulose at 2θ = 22.8, 14.6, and 17.7°, which were assigned to the planes of (200), (11̅0), and (110), respectively (Figure 2a). Notably, these intense peaks also demonstrated the high crystalline nature of the aerogel derived from bacterial cellulose, which was consistent with previous studies on cellulose obtained from bacterial fermentation. (29,36,37) The morphology of the aerogel sample was also observed through the SEM analysis (Figure 2b). The bacterial cellulose material consisted of fibers and bundles with diameters ranging from 20 to 50 nm. These bundles were irregularly arranged with a high degree of interconnection to form the 3D matrix due to the accidental appearances and movements of A. xylinum bacteria in the fermentation medium. (38)

Figure 2

Figure 2. Characterizations of the aerogel material derived from pineapple peel waste: PXRD pattern (a); SEM image (b); N2 physisorption isotherm (c); and pore size distribution (d).

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The porosity of the bacterial cellulose network was strongly dependent on the drying method for the removal of solvents, as previously reported in the literature. (39,40) In fact, a non-porous thin sheet was produced by employing thermal drying under atmospheric or reduced pressure to treat the hydrogel form of bacterial cellulose. Under such traditional drying approaches, water vapor was diffused throughout the cellulose matrix, leading to agglomeration of the fibers. In addition, abundant hydrogen bonding in the bacterial cellulose network could also accelerate the structural collapse. (40−43) Alternatively, freeze-drying and supercritical CO2 drying have been commonly used for the preparation of aerogels from bacterial cellulose due to the good preservation of the pristine 3D network. (43−46) Typically, using these as-prepared bacterial cellulose sources at a concentration of 0.40% in a two-minute ground suspension with water, the freeze-dried bacterial cellulose aerogel could be obtained with an average bulk density of 0.0051 ± 0.0003 g/cm3 which was determined based on 9 different samples. As expected, the aerogel presented a BET surface area of approx. 35 m2/g. The obtained isotherm for this sample can be classified as Type II according to the IUPAC classification for macroporous materials. However, a hysteresis loop at the relative pressure from 0.80 to 0.96 proved the appearance of both mesopores and macropores in the aerogel (Figure 2c). (47−50) The DFT-based pore size distribution indeed showed a wide range of pore sizes larger than 50 Å, which was attributed to the 3D bacterial cellulose network generated in nata de pina (Figure 2d). (40) Furthermore, FT-IR measurement was performed to identify the functional groups present in the aerogel (Figure S1). Accordingly, three characteristic stretching vibrations typically assigned to hydroxyl (O–H), methylene (−CH2−), and ether groups (C–O) of cellulose were, respectively, observed at 3342, 2894, and 1056 cm–1, respectively. (51,52) These electron-rich saturated oxygen atoms could attract cationic species in the aqueous phase. Meanwhile, the strong polarization of the hydroxyl group offers a potential platform for the formation of hydrogen bonds with the electronegative atoms in the dye molecules. Such electrostatic interactions could be responsible for the aqueous adsorption of organic dyes onto the aerogel surface.
The thermal stability of the bacterial cellulose aerogel prepared by freeze-drying at 0.5 mbar for 48 h was investigated via TGA. The profile was recorded from 30 to 900 °C under an air atmosphere. A minor weight loss of approx. 5% was observed up to 300 °C due to the release of moisture in the sample. Above 300 °C, the fresh BC sample was decomposed and combusted rapidly into COx and H2O, and the combustion was almost completed at 360 °C (Figure 3a). (53) The TGA analysis was also employed to discover the thermal behavior of the aerogel sample after the adsorption experiment with a 50-ppm solution of methylene blue for 30 min. It was observed that this TGA profile almost overlapped with that of the bare aerogel up to 300 °C, indicating a reassembling thermal behavior of the BC aerogel in both samples. However, a distinct difference in weight loss was observed for the samples from 300 to 490 °C. The slow rate of weight loss in the profile of the used aerogel sample was associated with the presence of methylene blue trapped in this adsorbent after the adsorption (Figure 3b). To further clarify the capture efficiency of the bacterial cellulose aerogel derived from pineapple peel waste for methylene blue, a series of experiments were carried out based on variations of the adsorption conditions including exposure time, initial concentration, temperature, and initial pH value of the methylene blue solution.

Figure 3

Figure 3. TGA profiles of the fresh BC aerogel (a) and the BC sample after the adsorption experiment with a 50-ppm solution of MB for 30 min (b).

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3.2. Adsorption Studies

First, the MB adsorption was carried out at different temperatures for 30 min to investigate its influence on the performance of the prepared material in trapping MB from the aqueous solution. As shown in Figure 4, the MB trapping capacity could reach up to 16 mg/g, corresponding to a removal efficiency (RE) of approximately 63.5% at 60 °C, and this value gradually decreased to 12.3 mg/g (RE ≈ 49.2%) as the adsorption process was carried out at 20 °C. This drop implied that capturing methylene blue from an aqueous solution by the BC aerogel derived from pineapple peel waste was an exothermic process. This could be caused by the formation of physical or chemical bonds between the active sites and adsorbates. (54−56)

Figure 4

Figure 4. Effect of temperature on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at pH = 6.5 for 30 min.

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In the next study, the effect of the adsorption time on the performance of the prepared aerogel was also investigated at various time intervals from 0 to 120 min at 30 °C (Figure 5). The trapping capacity rapidly increased to 14.7 mg/g (RE ≈ 58.9%) in the first 20 min of the adsorption, then the removal efficiency steadily rose and reached a saturation state after about 30 min. To clarify the adsorption kinetics of MB molecules into the cellulose framework, this time-dependent adsorption profile was further employed based on the pseudo-first-order and pseudo-second-order models (eqs 1 and 2). (33) The correlation coefficients were found to be 0.999 and 0.702 for the second-order and the first-order models, respectively (Figure 6), implying that the adsorption of MB on cellulose aerogel was better fitted with the pseudo-second-order model. Based on the previous reports, the rate-determining step in this adsorption process was related to both physical and chemical interactions, which could be attributed to the functional group present in the aerogel matrix and the MB molecule. Namely, the bacterial cellulose framework includes a large number of electron-rich saturated oxygen atoms in the hydroxyl (−OH) and ether (−O−) groups, while the cation in MB is not only positively charged but also possesses many nitrogen atoms with lone electron pairs. (33,52,57,58) Therefore, the adsorption of MB into the BC network could be assigned to different electrostatic interactions, i.e., the attraction force between the saturated oxygen atoms in cellulose and the cationic species and the hydrogen bonding of the hydroxyl hydrogen atoms with the nitrogen atoms in MB (Figure 7). (59−61)

Figure 5

Figure 5. Effect of adsorption time on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at 30 °C, and pH = 6.5.

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Figure 6

Figure 6. (a) First-order and (b) second-order adsorption kinetics of the methylene blue adsorption using the bacterial cellulose aerogel material.

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Figure 7

Figure 7. Proposal of adsorptive sites and their interactions with methylene blue molecules at different pH values.

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Since the adsorption process was based on electrostatic interactions, the initial pH of the aqueous solution might play an important role in the MB-trapping efficiency of the BC aerogel. (9) In other words, the removal of methylene blue could be impacted by the presence of guest ions, such as proton, hydroxide, or other charged species. (10,62) Therefore, the adsorption of methylene blue was then studied in the range of solution pH from 3 to 11. The result showed that increasing the pH was beneficial for the trapping of MB into the aerogel material (Figure 8). Particularly, the experiment at the initial pH of 6.5 afforded an adsorption capacity of approx. 14.8 mg/g (RE = 59.3%). The MB uptake was significantly reduced by half as the solution was further acidified to pH = 3.6. In contrast, only a minor activity enhancement of 10% occurred as the pH increased from 6.5 to 11.

Figure 8

Figure 8. Effect of the pH value on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at 30 °C for 30 min.

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To elucidate the pH-dependent adsorptive behavior of the aerogel, its zero-charge point (pHpzc) was also determined via the pH alteration in various solutions added with the aerogel. As shown in Figure S2, the entire surface charge of the cellulose material adsorbent is equal to zero at pH ≈ 7.3, close to the results previously obtained for the pure cellulose-based materials. (51,63) Therefore, the aerogel surface should be more positively charged under acidic conditions because the electron-rich oxygen atoms on cellulose chains would be facilely occupied by the H+ ions. Notably, Leyva-Ramos and co-workers previously described that methylene blue molecules exist in an aqueous solution as both cationic species and undissociated molecules. Its neutral form could occupy approx. 75% at pH = 3.6, while the cationic one appeared under less acidic conditions and could be the sole form at pH > 6. (64) Obviously, the access of the MB cationic species to the cellulose network might be significantly hindered due to the repulsive interaction between the same charges at the very low pH of 3.6. However, a minor amount of MB could be adsorbed under this condition, possibly based on the hydrogen bonding between nitrogen in MB and hydrogen of the unprotonated hydroxyl groups (Figure 7a). (10,55) In contrast, the solution basification induced the deprotonation of the hydroxyl groups, increasing the negative charge density of the aerogel surface. As a result, these negatively charged functional groups would strongly interact with the positively charged MB species (the dominant form of MB at pH > 6) via the proposed electrostatic interactions (Figure 7c). It should be noted that the deprotonation was likely insignificant under the applied conditions; therefore, only slight improvements in the MB-trapping efficiency were observed based on the pH increase. (65,66)
Varying the initial methylene blue concentration for the adsorption course in the range of 0–400 ppm was also conducted to determine the maximal adsorption capacity of this BC aerogel (Figure 9). The adsorption capacity for MB considerably increased from 4.1 to 29.7 mg/g with growth in the initial concentration of MB from 10 to 200 ppm, respectively. No further improvements in the removal capacity were observed for higher concentrations. As the solutions become more concentrated, the ratio of the adsorbates over open adsorptive centers increases, providing a stronger driving force for the adsorption of MB. (62) In contrast, in terms of the removal efficiency, 81% of MB was trapped by the BC aerogel at the low MB concentration, namely 10 ppm. Increasing the initial MB concentration led to a corresponding decrease in the MB removal percentage due to the MB excess in the solution. However, this progress was also controlled by the number of adsorptive sites. In other words, the adsorption efficiency of aerogel would reach the saturation state after all active centers, namely the hydroxyl groups and the rich-electron oxygen atoms on the cellulose backbone, were occupied by the methylene blue cations. (10,67) Therefore, concentrations higher than 200 ppm cannot provide more dynamics to further improve MB trapping.

Figure 9

Figure 9. Effect of initial methylene blue concentration on adsorption capacity. Adsorption condition: 20 mg of aerogel, 10 mL of MB solution at 30 °C for 30 min and pH = 6.5.

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These initial concentration-dependent adsorption results were employed to continuously investigate the adsorption mechanism of the MB on the cellulose surface using the Langmuir and Freundlich equations (eqs 3 and 4). In detail, the Langmuir model assumes monolayer coverage of adsorbate onto a homogeneous adsorbent, while the Freundlich one hypothesizes reversible adsorption including both formations of monolayer and multilayer of adsorbates. (55,57,68) It was observed that the MB adsorption isotherm data of aerogel material derived from pineapple peel waste fit better to the Langmuir model with a high correlation coefficient of 0.996, than the Freundlich equation which had a low correlation coefficient of 0.934 (Figure 10). In addition, the maximal adsorption capacity for MB determined by the Langmuir model was approx. 31.1 mg/g, very close to the experimental result recorded at the high MB concentrations. In other words, the adsorption of MB molecules likely carried out and generated one adsorbate molecular layer onto the fixed active sites of cellulose fibers. And, there was no interaction between the adsorbed molecules, including neighboring sites. (68,69)

Figure 10

Figure 10. MB adsorption isotherms of the BC aerogel derived from pineapple peel waste fitted by Langmuir model (a) and Freundlich model (b).

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The aerogel preparation conditions also impacted the MB adsorption efficiency due to their effect on the formation of the BC matrix. Accordingly, different concentrations of BC in water from 0.24 to 0.80 wt % were prepared after 2 min grinding. Subsequently, freeze-drying was carried out, yielding five corresponding aerogel samples. As shown in Figure 11a, increasing the cellulose content in the suspension phase led to significant increases in the as-prepared aerogel density; however, large drops (up to 40%) in the surface area were observed. Interestingly, only minor losses (1–10%) in the adsorption efficiency of the BC aerogel were recorded, indicating a weak correlation between the aerogel’s performance and its porosity (Figure 11b). It was based on the fact that BC aerogels can undergo hydration in the aqueous phase, thereby further changing the pristine aerogel structure.

Figure 11

Figure 11. Photographs of aerogel samples prepared from the suspensions with varied BC concentrations (a) and their effect on the adsorption capacity and the specific surface area of the obtained aerogels (b).

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Furthermore, the effect of the nata de pina size on the aerogel texture and its adsorption performance was investigated. In detail, the grinding time of the nata de pina/water mixture was varied from 1 to 5 min to obtain different particle sizes of nata de pina before the suspension phases were prepared at the same BC concentration of 0.40 wt % for freeze drying. This provided another series of five BC aerogel samples. It should be observed that grinding was essential to obtain the BC aerogel. Freeze-drying the pristine nata de pina sample in 1 cm cubes indeed yielded thin sheets with negligible porosity and adsorption capacity for MB. The BC frameworks in this form needed to be fragmented and interleaved with others by grinding, which was followed by freeze-drying, affording a desired aerogel structure. As can be predicted, prolonging grinding considerably reduced the nata de pina size; however, the density of the obtained BC aerogels remained almost unchanged with no significant alterations detected (Table 2), proving that the obtained aerogel texture was independent of the nata de pina size within the studied time range of grinding. Therefore, the MB trapping capacities were recorded at approx. 30 mg/g for all of the samples observed (Figure 12).

Figure 12

Figure 12. Methylene blue adsorption capacity on the aerogel samples prepared from the suspensions with different sizes of nata de pina hydrogel particles. Adsorption condition: 20 mg of aerogel, 10 mL of MB solution with a concentration of 200 ppm, at 30 °C for 30 min and pH = 6.5.

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Table 2. Bacterial Cellulose Aerogels Prepared From the Suspensions With Different Grinding Times
Grinding time (min)12345
Median size of nata de pina (μm)982.2670.4633.3565.0414.0
Density of the obtained aerogel (g/cm3)0.00510.00510.00500.00570.0052
In the last two decades, various plant-based cellulose waste sources, such as bagasse, sawdust, sugar beet pulp, cotton, and sago pith, have been recycled for the adsorption of MB. In general, complicated chemical treatments were required for the removal of lignin and other impurities which can affect the textural properties of the desired adsorbent as well as prevent the functional groups on the cellulose fiber from further chemical modification or interaction with the adsorbate species. Using the adsorbent derived from plant cellulose, the MB uptake was reported to be in a broad range of 1.4–42.2 mg/g, depending on the material type and composition and adsorption conditions (entries 1–10, Table 3). On the other hand, modification of the cellulose surface and combination with other materials have recently allowed significant improvements in the adsorption activity (Entries 11–14, Table 3). Although a high adsorption capacity could be obtained using the modified cellulose-based biosorbents, the practical application of these materials might be limited due to the tremendous consumption of energy and chemicals for material purification and preparation. Bacterial cellulose-based adsorbents, therefore, offer many notable advantages, including viable production, high purity, facile pre-treatment, and no required toxic chemicals. (61,70) More importantly, in this study, it can be highlighted that the bacterial cellulose aerogel derived from the pineapple peel waste showed a comparable efficiency of 29.6 mg/g in capturing methylene blue from an aqueous solution without any further chemical functionalization (entry 15, Table 3). In addition, valorization strategies for fruit and vegetable wastes should be implemented to reduce disposal costs and environmental effects. (71) Therefore, the utilization of pineapple peel for the preparation of bacterial cellulose for water treatment could be considered a promising sustainable approach to raise the economic value of this abundant waste.
Table 3. MB Adsorption Capacity of Different Cellulose-Based Materials
EntryMaterialAdsorption conditionsAdsorption capacity (mg/g)Refs
1Cetyltrimethylammonium bromide-modified carboxymethyl cellulose/bagasse cryogelpH = 7, 25 °C, Co = 5 ppm, dose = 100 mg/3 mL, 60 min1.4 (72)
2Oxidized cellulose nanofibers/polyvinyl alcohol/montmorillonite K-10 composite aerogel25 °C, Co = 20 ppm, dose = 400 mg/50 mL, 25 min2.3 (58)
3Hydroxypropyl cellulose/graphene oxide hydrogel25 °C, Co = 80 ppm, dose = 190 mg/100 mL, 10 h11.5 (73)
4Carboxymethyl cellulose/k-carrageenan/activated montmorillonite composite beadpH = 6, 30 °C, Co = 25 ppm, dose = 100 mg/50 mL, 300 min12.4 (74)
5Hydrolyzed wheat strawpH = 8, 23 °C, Co = 14 ppm, dose = 500 mg/500 mL, 280 min16.2 (75)
6Magnetite/phenylenediamine/cellulose acetate nanocompositepH = 6, 25 °C, Co = 50 ppm, dose = 30 mg/20 mL, 70 min29 (76)
7Magnetic cellulose/graphene oxide compositepH = 6, 25 °C, Co = 30 ppm, dose = 50 mg/50 mL, 14 h29.5 (77)
8Porous cellulose microbead derived from waste cotton treated with NaOH/ureapH = 7, 25 °C, Co = 100 ppm, dose = 1 g/50 mL, 120 min32.5 (74)
9Sawdust-based cellulose/ZnO nanocompositepH = 7, 25 °C, Co = 150 ppm, dose = 100 mg/50 mL, 300 min42 (78)
10Poly(acrylic acid)/nanocrystalline cellulose nanocomposite hydrogelambient temperature, pH = 8, Co = 5 ppm, dose = 50 mg/100 mL, 120 min42.2 (79)
11Cellulose acetate/polydopamine composite nanofiber membranepH = 6.5, 25 °C, Co = 50 ppm, dose = 10 mg/20 mL, 24 h88.2 (80)
12Sugar beet pulp cellulose/sodium alginate/iron hydroxide composite hydrogelpH = 6.5, 25 °C, Co = 200 ppm, dose = 30 mg/25 mL, 150 min93 (81)
13Carboxylated cellulose25 °C, Co = 35 ppm, dose = 100 mg/10 mL, 1.5 h97.5 (82)
14Cellulose nanofibril-based aerogel derived from sago pith wastepH = 7, 20 °C, Co = 90 ppm, dose = 5 mg/20 mL, 40 min222.2 (83)
15Bacterial cellulose aerogel derived from pineapple peel wastepH = 6.5, 30°C, Co = 200 ppm, dose = 20 mg/10 mL, 30 min29.7this study
This study was also expanded to various cationic and anionic dyes with the results shown in Figure 13. Similar to methylene blue, other positively charged dye species derived from rhodamine B, crystal violet, and malachite green could be adsorbed by the BC aerogels due to the electron-rich oxygen atoms abundantly present in cellulose. Approximate adsorption capacities (30 mg/g) for methylene blue, rhodamine B, and crystal violet were recorded while malachite green was adsorbed with a 50% higher amount (48.6 mg/g) under identical conditions. It should be noticed that malachite green was relatively as large as crystal violet but larger than methylene blue (Table 1). Therefore, it was suggested that the removal of cationic organic dyes by the BC aerogel material was independent of their molecular size. And this process could be determined by the nature of functional groups on organic compounds, which offered various chemical interactions to adsorptive sites onto the cellulose backbone. By contrast, the BC aerogel was inefficient for the anionic species of sunset yellow, quinoline yellow, and methyl orange, while the sizes of these compounds were similar to that of methylene blue (Table 1). This could be rationalized by the inactivity or the repulsion of the electron-rich oxygen atoms onto the cellulose backbone in anionic organic dyes. Notably, an exceptional case was observed for congo red, which is also classified as an anionic organic dye. A gram of BC aerogel can adsorb up to 101.4 mg of congo red, which was significantly higher than the cationic dyes recorded in this study. It should be noted that the congo red molecule possesses two more amine groups besides the typical sulfonate moieties of the anionic dye class. Therefore, the hydrogen bonding-based interaction of these amine groups with the hydroxyl groups of cellulose could be responsible for such impressive uptake of congo red on the BC aerogel. According to Chong and co-authors, the possible formation of hydrogen bonding between hydroxyl groups of the cellulose aerogel and various hydrogen bond acceptors on the congo red backbone, including aromatic rings, nitrogen, sulfur, and oxygen atoms, could be considered as a rational reason for the impressive adsorption capacity. (84,85) However, further studies are still needed for a better understanding of the high selectivity of aerogel materials derived from cellulose frameworks toward the congo red molecules.

Figure 13

Figure 13. Adsorption capacity of the aerogel for various organic dyes. Adsorption condition: 20 mg of aerogel, 10 mL of dye solution with a concentration of 200 ppm, at 30 °C and pH = 6.5 for 30 min.

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To further discover the adsorption selectivity of the bacterial cellulose aerogel toward cationic and anionic dyes, an adsorption experiment was performed with a solution containing quinoline yellow (anionic dye) and methylene blue (cationic dye). The adsorption of the dyes was monitored by withdrawing aliquots from the solution at different time intervals for UV–vis spectroscopy. The initial solution exhibited two absorbance peaks at 441 and 664 nm, indicating the presence of these anionic and cationic dyes. As can be predicted, there was a significant drop in the intensity of the 664 nm peak within only 1 min of contact with the aerogel while the 441 nm peak remained almost unchanged during the 30 min experiment (Figure S3). The different adsorption behavior between MB and QY with the BC aerogel indeed proved the high affinity of the electron-rich bacterial cellulose surface with the positively charged species. On the other hand, the repulsive interaction between the aerogel and the anions was dominant, resulting in the inefficiency of trapping the anionic dyes. However, the introduction of amine groups to the dye anions, e.g., congo red, could improve the attraction toward the cellulose matrix via the formation of hydrogen bonding on the cellulose surface.
Notably, the adsorption for MB was scaled up to 5–50 times larger batches by increasing the adsorption volume while keeping the same ratio of adsorbent/solution. The result showed that the MB trapping capacity was in a range from 29.2 to 29.8 mg/g for all tested scales from 10 to 500 mL, indicating that there was no mass transfer limitation in the adsorption even scaling up 50 times (Figure 14). These results demonstrated that the bacterial cellulose-based material prepared in this work would be a promising ideal platform for the removal of harmful chemicals from an aqueous solution.

Figure 14

Figure 14. Effect of aqueous solution volume on methylene blue adsorption capacity of the aerogel and recycling test employing cellulose-based aerogel in the removal of methylene blue (*). Adsorption condition: solid/liquid ratio = 2 mg/1 mL with a concentration of 200 ppm MB, at 30 °C and pH = 6.5 for 30 min.

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The recovery and reuse of adsorbents are one of the most important objectives toward zero waste in practical processes. (61) In this study, the recyclability of the MB-saturated aerogel was carried out by washing with different solvents. The used aerogel was isolated after a 30 min adsorption experiment. Three pure single solvents, including water, ethanol, and acetone, in which MB is well soluble, were used to wash MB from the spent aerogel. However, the complete removal of MB was unsuccessful as the MB molecules were durably trapped in the BC matrix upon chemical interactions, even though a large amount of these solvents was applied (Figure S4a–c). Alternatively, based on the fact that the MB adsorption was poor under acidic conditions, an acid-containing solution, namely, 5 wt % HCl in acetone was applied. It was observed that the MB species absorbed in the aerogel were efficiently washed out with this acidic solution as the adsorbent turned back to its original white color (Figure S4d). This could be explained by the fact that the trapped cationic species were facilely exchanged with protons in the acidic solution. Moreover, a proton excess might prevent the re-adsorption of MB at the adsorptive sites of the BC backbone. The resulting solid was subsequently washed three times with water until neutralization, prior to freeze-drying to reproduce the aerogel form (Figure S5). Characterization of the regenerated aerogel by XRD, FT-IR, and SEM showed that no significant structural alterations had occurred (Figure S6). Indeed, the three-dimensional crystalline framework of bacterial cellulose in the recycled aerogel was maintained in comparison to the fresh one. However, approx. 5% of the initial aerogel mass was lost possibly due to acidic hydrolysis. The spent bacterial cellulose-based material was reused for a new cycle of the MB adsorption experiment under identical conditions at the 500 mL scale. As shown in Figure 14, the MB-trapping efficiency decreased by approx. 14%. This decrease in the adsorption capacity was partially attributed to the aerogel loss during regeneration. The result also indicated that another fraction of about 9% of the adsorption sites was not recovered through regeneration. Therefore, it would be concluded that the used aerogel from the adsorption of MB can be partially regenerated; however, complete regeneration is still challenging and requires further study.

4. Conclusions

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In this work, nata de pina obtained from the bacterial fermentation of pineapple water was employed as the cost-efficient bacterial cellulose source to produce highly crystallite and ultralight aerogels via the freeze-drying technique. These aerogels have a 3D network with large pores derived from the unordered interconnection of cellulose fibers and a high density of the hydroxyl group on the surface, which could efficiently adsorb cationic dyes and a selected anionic dye. The cellulose content (0.24–0.80%) in the aerogel materials only showed a modest impact on capturing methylene blue, while the adsorption conditions, including exposure time, temperature, initial pH value, and concentration of the solution significantly affected the adsorption performance. A remarkable MB uptake of 29.7 mg/g was found at 30 °C, pH = 6.5 for 30 min. The adsorption of methylene blue onto cellulose aerogels was fast and fit well with the pseudo-second-order and Langmuir adsorption models. Besides, the aerogel derived from bacterial cellulose also exhibited remarkable selective removal of different cationic dyes, including rhodamine B, crystal violet, and malachite green, with adsorption capacities of 28.0, 33.0, and 48.6 mg/g, respectively, due to a strong interaction between the positive charge of these cation dyes with the negative charge of the hydroxyl group on the surface of the cellulose aerogels. By contrast, no uptakes were recorded for most of the anionic dyes, namely methyl orange, sunset yellow, and quinoline yellow, because of repulsion between the two negative charges of the dyes and the adsorbents. However, an exception for one anionic dye─congo red─was recorded, in which the cellulose aerogels showed a substantially high adsorption capacity (101.4 mg/g) due to a strong hydrogen bond between the cellulose aerogels and the two amine groups of red congo. More importantly, the aerogel materials exhibited the same performance in up-scaling conditions of 5–50 times.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsomega.3c03130.

  • FTIR spectrum of fresh cellulose-based aerogel; determination of the zero-charge point (pHPZC) of the cellulose-based aerogel; UV–vis absorption spectra of the mixture of quinoline yellow and methylene blue (200 ppm:200 ppm) in the presence of cellulose-based aerogel at 30 °C and pH = 6.5; photographs of the collected samples after washing three times different solvents such as water, ethanol, acetone, and acetone solution containing 5 wt % of HCl; photographs of the regenerated aerogel after freeze-drying; and characterization of the used cellulose-based aerogel after the adsorption (PDF)

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Author Information

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  • Corresponding Authors
    • Khoa Dang Nguyen - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam;  Email: [email protected]
    • Hanh Huynh Mai Nguyen - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam;  Email: [email protected]
    • Phuoc Hoang Ho - Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg SE-412 96, Sweden;  Orcidhttps://orcid.org/0000-0001-8571-4114;  Email: [email protected]
  • Authors
    • Ha Vu Le - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    • Nghia Thi Dao - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    • Ha Truc Bui - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
    • Phung Thi Kim Le - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam;  Orcidhttps://orcid.org/0000-0003-0570-3154
    • Kien Anh Le - Institute for Tropical Technology and Environmental Protection, 57A Truong Quoc Dung, Phu Nhuan District, Ho Chi Minh City 726500, Viet Nam
    • An Thi Tuong Tran - Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet Street, District 10, Ho Chi Minh City 740010, Viet Nam;  Vietnam National University Ho Chi Minh City, Linh Trung Ward, Thu Duc District, Ho Chi Minh City 740010, Viet Nam
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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This research is funded by Ho Chi Minh City University of Technology (HCMUT), VNU-HCM under grant number SVKSTN-2022-KTHH-10.

References

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    Removal of inorg. and org. pollutants from synthetic and industrial wastewater samples is one of the biggest challenges facing researchers. In this work, glycine-β-cyclodextrin-functionalized carbon nanotubes (MWCNTs/Gly/β-CD) as a novel nano-adsorbent were synthesized and developed for the removal of org. pollutants. The structure and morphol. of MWCNTs/Gly/β-CD was characterized by FT-IR, FESEM, TEM, XRD and EDX, and the results showed that the MWCNT was modified with Gly and β-CD. The effects of surface improvement on the adsorption of org. pollutants were studied in a batch system by considering various parameters such as contact time, adsorbent dosage, pH, and temp. The results indicated that the max. capacities of MB, AB113, MO and DR1 onto MWCNTs/Gly/β-CD were 90.90mg g-1, 172.41mg g-1, 96.15mg g-1, and 500mg g-1, resp. The dye adsorption kinetics, thermodn. and isotherms were also investigated. The results indicated that pseudo-second-order kinetics model (R2 > 0.999) and Langmuir isotherm model (R2 > 0.995) well describe the adsorption of the tested dyes on the MWCNTs/Gly/β-CD. In comparison with the raw MWCNTs and MWCNTs/Gly samples, the dye removal efficiency was increased for the synthesized MWCNTs/Gly/β-CD nano-adsorbent. Our results confirmed that β-CD-functionalized MWCNTs can be used as an effective adsorbent due to the high adsorption capacity of dyes as well as the short equil. time needed. Therefore, MWCNTs/Gly/β-CD was successfully applied to remove org. pollutants from synthetic and industrial wastewater samples with excellent results.
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  9. 9
    Xiao, W.; Jiang, X.; Liu, X.; Zhou, W.; Garba, Z. N.; Lawan, I.; Wang, L.; Yuan, Z. Adsorption of organic dyes from wastewater by metal-doped porous carbon materials. J. Cleaner Prod. 2021, 284, 124773,  DOI: 10.1016/j.jclepro.2020.124773
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    Adsorption of organic dyes from wastewater by metal-doped porous carbon materials
    Xiao, Wei; Jiang, Xingpeng; Liu, Xi; Zhou, Weiming; Garba, Zaharaddeen N.; Lawan, Ibrahim; Wang, Liwei; Yuan, Zhanhui
    Journal of Cleaner Production (2021), 284 (), 124773CODEN: JCROE8; ISSN:0959-6526. (Elsevier Ltd.)
    A review. In this review paper, the recent development on the adsorption of org. dyes by metal-doped porous carbon materials were reviewed. The primary objective of this paper is to sort out the dispersion information of metal-doped porous carbon materials widely used in org. dye adsorption. Various metal-doped porous carbon materials adsorbing org. dyes are summarized and discussed here for the first time. Key factors affecting the adsorption process such as the amt. of doped metal, soln. pH, and temp. are also reported and discussed. The adsorption mechanisms such as electrostatic interaction, π-π interaction, hydrogen bonding and synergistic interaction between metal particles and carbon materials are proposed for org. dyes adsorption on metal-doped porous carbon with the help of related works from the literature. Finally, few suggestions for future studies on metal-doped porous carbon materials are proposed.
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  10. 10
    Nguyen, K. D.; Ho, P. H.; Vu, P. D.; Pham, T. L. D.; Trens, P.; Di Renzo, F.; Phan, N. T. S.; Le, H. V. Efficient Removal of Chromium(VI) Anionic Species and Dye Anions from Water Using MOF-808 Materials Synthesized with the Assistance of Formic Acid. Nanomaterials 2021, 11, 1398,  DOI: 10.3390/nano11061398
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    10
    Efficient removal of chromium(VI) anionic species and dye anions from water using mof-808 materials synthesized with the assistance of formic acid
    Nguyen, Khoa D.; Ho, Phuoc H.; Vu, Phuong D.; Pham, Thuyet L. D.; Trens, Philippe; Renzo, Francesco Di; Phan, Nam T. S.; Le, Ha V.
    Nanomaterials (2021), 11 (6), 1398CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
    This study presents a simple approach to prep. MOF-808, an ultra-stable Zr-MOF constructed from 6-connected zirconium clusters and 1,3,5-benzene tricarboxylic acid, with tailored particle sizes. Varying the amt. of formic acid as a modulator in the range of 200-500 equiv results in MOF-808 materials with a crystal size from 40 nm to approx. 1000 nm. Apart from the high sp. surface area, a combination of a fraction of mesopore and plenty of acidic centers on the Zr-clusters induces a better interaction with the ionic pollutants such as K2Cr2O7 and anionic dyes. MOF-808 shows uptakes of up to 141.2, 642.0, and 731.0 mg/g for K2Cr2O7, sunset yellow, and quinoline yellow, resp., in aq. solns. at ambient conditions. The uptakes for the ionic dyes are significantly higher than those of other MOFs reported from the literature. Moreover, the adsorption capacity of MOF-808 remains stable after four cycles. Our results demonstrate that MOF-808 is a promising ideal platform for removing oxometallates and anionic dyes from water.
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    Hashim, M. A.; Mukhopadhyay, S.; Sahu, J. N.; Sengupta, B. Remediation technologies for heavy metal contaminated groundwater. J. Environ. Manage. 2011, 92, 2355– 2388,  DOI: 10.1016/j.jenvman.2011.06.009
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    Remediation technologies for heavy metal contaminated groundwater
    Hashim, M. A.; Mukhopadhyay, Soumyadeep; Sahu, Jaya Narayan; Sengupta, Bhaskar
    Journal of Environmental Management (2011), 92 (10), 2355-2388CODEN: JEVMAW; ISSN:0301-4797. (Elsevier Ltd.)
    A review. The contamination of groundwater by heavy metal, originating either from natural soil sources or from anthropogenic sources is a matter of utmost concern to the public health. Remediation of contaminated groundwater is of highest priority since billions of people all over the world use it for drinking purpose. In this paper, thirty five approaches for groundwater treatment have been reviewed and classified under three large categories viz chem., biochem./biol./biosorption and physico-chem. treatment processes. Comparison tables have been provided at the end of each process for a better understanding of each category. Selection of a suitable technol. for contamination remediation at a particular site is one of the most challenging job due to extremely complex soil chem. and aquifer characteristics and no thumb-rule can be suggested regarding this issue. In the past decade, iron based technologies, microbial remediation, biol. sulfate redn. and various adsorbents played versatile and efficient remediation roles. Keeping the sustainability issues and environmental ethics in mind, the technologies encompassing natural chem., bioremediation and biosorption are recommended to be adopted in appropriate cases. In many places, two or more techniques can work synergistically for better results. Processes such as chelate extn. and chem. soil washings are advisable only for recovery of valuable metals in highly contaminated industrial sites depending on economical feasibility. Various technologies for remediating heavy metal contaminated groundwater has been reviewed.
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  12. 12
    Gupta, V. K.; Carrott, P. J. M.; Ribeiro Carrott, M. M. L.; Suhas Low-Cost Adsorbents: Growing Approach to Wastewater Treatment─a Review. Crit. Rev. Environ. Sci. Technol. 2009, 39, 783– 842,  DOI: 10.1080/10643380801977610
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    Wolok, E.; Barafi, J.; Joshi, N.; Girimonte, R.; Chakraborty, S. Study of bio-materials for removal of the oil spill. Arabian J. Geosci. 2020, 13, 1244,  DOI: 10.1007/s12517-020-06244-3
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    Khamkeaw, A.; Jongsomjit, B.; Robison, J.; Phisalaphong, M. Activated carbon from bacterial cellulose as an effective adsorbent for removing dye from aqueous solution. Sep. Sci. Technol. 2018, 54, 2180– 2193,  DOI: 10.1080/01496395.2018.1541906
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    Maleki, H. Recent advances in aerogels for environmental remediation applications: A review. Chem. Eng. J. 2016, 300, 98– 118,  DOI: 10.1016/j.cej.2016.04.098
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    Recent advances in aerogels for environmental remediation applications: A review
    Maleki, Hajar
    Chemical Engineering Journal (Amsterdam, Netherlands) (2016), 300 (), 98-118CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
    A review concerning recent advances in aerogel synthesis, processing, and air and water purifn. adsorption applications is given. Topics discussed include: introduction; synthesis (sol-gel process, aging, drying [supercrit., ambient pressure, freeze], carbonization, carbo-thermal redn. to prep. carbide aerogels); aerogel air purifn. applications (CO2 capture, volatile org. compd. removal); aerogel water purifn. applications (oil and toxic org. pollutant clean-up, heavy metal ion removal); and conclusions and outlook. Although, aerogel environmental remediation performance is promising, some drawbacks (an intricate drying process, mech. delicate structure, processing cost) were examd. and were abated in some manner in several studies.
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    Wang, Y.; Su, Y.; Wang, W.; Fang, Y.; Riffat, S. B.; Jiang, F. The advances of polysaccharide-based aerogels: Preparation and potential application. Carbohydr. Polym. 2019, 226, 115242,  DOI: 10.1016/j.carbpol.2019.115242
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    The advances of polysaccharide-based aerogels: Preparation and potential application
    Wang, Yixin; Su, Yuehong; Wang, Weiling; Fang, Ying; Riffat, Saffa B.; Jiang, Fatang
    Carbohydrate Polymers (2019), 226 (), 115242CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
    A review. Polysaccharide-based aerogels have high application value as one kind of unique functional materials. Not only has it high porosity and low-d., but also the non-toxicity and biodegradability. In recent decades, a variety of natural raw materials and their combinations along with various prepn. technologies have been investigated to develop polysaccharide-based aerogels with different functions for diverse applications. This review aims to clarify a general approach in the development of polysaccharide-based aerogels regarding pore structure design, polysaccharide selection and drying methods. The relevant researches and reports of polysaccharide-based aerogels have been also classified according to the applications in environmental engineering, buildings, medical practice, packaging and electrochem. Furthermore, some statistical graphs have been produced to summarize those publications during the past ten years, with an aim to indicate the distribution and research trend. Finally, the approaches to improve the quality of the aerogels are discussed and some perspectives are put forward to provide a ref. for the future development of polysaccharide-based aerogels.
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    Chen, X.; Cui, J.; Xu, X.; Sun, B.; Zhang, L.; Dong, W.; Chen, C.; Sun, D. Bacterial cellulose/attapulgite magnetic composites as an efficient adsorbent for heavy metal ions and dye treatment. Carbohydr. Polym. 2020, 229, 115512,  DOI: 10.1016/j.carbpol.2019.115512
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    Bacterial cellulose/attapulgite magnetic composites as an efficient adsorbent for heavy metal ions and dye treatment
    Chen, Xiao; Cui, Jian; Xu, Xuran; Sun, Bianjing; Zhang, Lei; Dong, Wei; Chen, Chuntao; Sun, Dongping
    Carbohydrate Polymers (2020), 229 (), 115512CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
    In recent decades, increased industrial activities led to the release of various pollutants, such as toxic heavy metals, inorg. anions, and orgs. It is imperative but challenging to develop an eco-friendly treatment technol. with easy operation, low cost, and high efficiency. Here, we describe a design of magnetic purifier, which has biomass-based structure by blending attapulgite/chitosan (ATP/CS) composite with bacterial cellulose nanofibrils (BCNs). Compared to similar materials reported previously, the product exhibited efficient adsorption capacities towards various metal ions including Pb2+, Cu2+, and Cr6+, and anionic org. dyes including Congo red. The adsorption process could be well fitted by Langmuir isotherm and pseudo-second order equation. Addnl., the adsorption capacity only decreased <8% after 5 adsorption-desorption cycles. We expect the design will inspire more efforts to build a multifunctional H2O purifier with simple operation, and hopefully effectively remove pollutants from wastewater in future practical applications.
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    Budtova, T. Cellulose II aerogels: a review. Cellulose 2019, 26, 81– 121,  DOI: 10.1007/s10570-018-2189-1
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    Cellulose II aerogels: a review
    Budtova, Tatiana
    Cellulose (Dordrecht, Netherlands) (2019), 26 (1), 81-121CODEN: CELLE8; ISSN:0969-0239. (Springer)
    A review. Cellulose II aerogels are light-wt., open pores materials with high sp. surface area. They are made in the same way as bio-aerogels based on other polysaccharides, via dissoln.-(gelation)-solvent exchange-drying with supercrit. CO2. Gelation step is often omitted as cellulose allows keeping 3D shape during solvent exchange (which leads to cellulose coagulation) and drying. Drying in supercrit. conditions preserves the porosity of "wet" (coagulated) cellulose. There are numerous ways to vary cellulose II aerogel morphol. and properties by changing processing conditions and cellulose type. Together with chem. and phys. modifications of cellulose and possibility of making hybrid and composite materials (org.-inorg. and org.-org.), it opens up a huge variety of aerogel properties and applications. On one hand, they are similar to those of classical aerogels, i.e. can be used for absorption and adsorption, as catalysts and catalysts support and in electro-chem. when pyrolyzed. On the other hand, because the prepn. of cellulose aerogels may not involve any toxic compds., they can be used in life science applications such as pharma, bio-medical, food and cosmetics. The review makes an overview of results reported in literature on the structure and properties of cellulose II aerogels and their applications. The reader may be surprised finding more questions than answers and clear trends. The review shows that several fundamental questions still remain to be answered and applications to be explored.
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    Galiwango, E.; Abdel Rahman, N. S.; Al-Marzouqi, A. H.; Abu-Omar, M. M.; Khaleel, A. A. Isolation and characterization of cellulose and α-cellulose from date palm biomass waste. Heliyon 2019, 5, e02937  DOI: 10.1016/j.heliyon.2019.e02937
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    Wang, N.; Xu, B.; Wang, X.; Lang, J.; Zhang, H. Chemical and Structural Elucidation of Lignin and Cellulose Isolated Using DES from Bagasse Based on Alkaline and Hydrothermal Pretreatment. Polymers 2022, 14, 2756,  DOI: 10.3390/polym14142756
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    Chemical and Structural Elucidation of Lignin and Cellulose Isolated Using DES from Bagasse Based on Alkaline and Hydrothermal Pretreatment
    Wang, Na; Xu, Baoming; Wang, Xinhui; Lang, Jinyan; Zhang, Heng
    Polymers (Basel, Switzerland) (2022), 14 (14), 2756CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
    The sepn. of cellulose, hemicellulose, and lignin components using deep eutectic solvent, which is a green solvent, to obtain corresponding chems. can realize the effective sepn. and high-value utilization of these components at low cost. In this study, we used waste biomass sugarcane bagasse as the raw material, choline chloride as the hydrogen bond acceptor, and lactic acid as the hydrogen bond donor to synthesize a deep eutectic solvent of choline chloride/lactic acid (L-DES) and treated sugarcane bagasse pretreated by alkali or hydrothermal methods to sep. cellulose, hemicellulose, and lignin. In addn., we comparatively studied the effect of different pretreatment methods on lignin removal by DES and found that the lignin removal rate by L-DES after alk. pretreatment was significantly higher than that after hydrothermal pretreatment, and the mechanism of action causing this difference is discussed.
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    Rehman, N.; Alam, S.; Amin, N. U.; Mian, I.; Ullah, H. Ecofriendly Isolation of Cellulose from Eucalyptus lenceolata: A Novel Approach. Int. J. Polym. Sci. 2018, 2018, 8381501– 7,  DOI: 10.1155/2018/8381501
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    Urbina, L.; Corcuera, M. Á.; Gabilondo, N.; Eceiza, A.; Retegi, A. A review of bacterial cellulose: sustainable production from agricultural waste and applications in various fields. Cellulose 2021, 28, 8229– 8253,  DOI: 10.1007/s10570-021-04020-4
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    A review of bacterial cellulose: sustainable production from agricultural waste and applications in various fields
    Urbina, Leire; Corcuera, Maria Angeles; Gabilondo, Nagore; Eceiza, Arantxa; Retegi, Alona
    Cellulose (Dordrecht, Netherlands) (2021), 28 (13), 8229-8253CODEN: CELLE8; ISSN:0969-0239. (Springer)
    A review. Bacterial cellulose (BC) is a polymer with interesting conformation and properties. BC can be obtained in different shapes and is easily modified by chem. and phys. means, so its applications in the prodn. of new materials and nanocomposites for different purposes have been in the focus of many research projects. However, one of the major challenges to address in bacterium-derived polymer technol. is to find suitable carbon sources as substrates that are cheap and do not compete with food prodn. for achieving large scale industrial applications. Agricultural wastes are defined as the residues from the growing and processing of raw agricultural products such as crops, fruits, vegetables and dairy products. Their compn. can vary depending on the type of agricultural activity and harvesting conditions, but these residues are suitable for the prodn. of BC. The aim of this review is to give insight into the prodn. of BC using agro-wastes and an overview of the most interesting and novel applications of this biopolymer in different areas i.e. environmental applications, optoelectronic and conductive devices, food ingredients and packaging, biomedicine, and 3D printing technol.
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    Anwar, B.; Bundjali, B.; Arcana, I. M. Isolation of Cellulose Nanocrystals from Bacterial Cellulose Produced from Pineapple Peel Waste Juice as Culture Medium. Procedia Chem. 2015, 16, 279– 284,  DOI: 10.1016/j.proche.2015.12.051
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    Isolation of Cellulose Nanocrystals from Bacterial Cellulose Produced from Pineapple Peel Waste Juice as Culture Medium
    Anwar, Budiman; Bundjali, Bunbun; Arcana, I. Made
    Procedia Chemistry (2015), 16 (), 279-284CODEN: PCRHBG; ISSN:1876-6196. (Elsevier B.V.)
    Cellulose nanocrystals (CNC) were isolated by the sulfuric acid hydrolysis of bacterial cellulose (BC) produced by Gluconacetobacter xylinus using pineapple peel waste juice as culture medium. Optimal conditions of the acid hydrolysis were obtained at concn. of sulfuric acid of 50%, hydrolysis time ranging 25∼40 min and temp. at 50 °C. The FTIR study shows that the CNC spectrum were similar with BC which indicated that both have similar chem. compn.; however there are some peaks alteration at 2900 cm-1 and 1430 cm-1 which indicated that BC has changed into CNC. The crystallinity of CNC detd. by FTIR was found to be higher than BC. By TEM observation, the CNC particles had av. length of 325 nm and diam. of 25 nm with av. aspect ratio (L/D) around 13. The TEM images also show the morphol. of CNC that has rod-like structure.
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    Raghav, N.; Sharma, M. R.; Kennedy, J. F. Nanocellulose: A mini-review on types and use in drug delivery systems. Carbohydr. Polym. Technol. Appl. 2021, 2, 100031,  DOI: 10.1016/j.carpta.2020.100031
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    Nanocellulose: A mini-review on types and use in drug delivery systems
    Raghav, N.; Sharma, Manishita R.; Kennedy, John F.
    Carbohydrate Polymer Technologies and Applications (2021), 2 (), 100031CODEN: CPTACM; ISSN:2666-8939. (Elsevier Ltd.)
    A review. Development of effective drug delivery systems by the exploitation of biocompatible, inert nanomaterials has become the thrust areas of research in medicinal chem. Out of various materials of significance, one is nanocryst. cellulose due to its biocompatibility and inertness. Further its surface modification can also be accomplished using variety of methods. In the present review we have compiled different types of nanocellulose and their use as drug delivery systems. The review recapitulate the literature not reported in recent reviews of 2019 and 2020. The review is focused on method of prepn. of nanocellulose and its application in oral, transdermal and local drug delivery systems. Limitations and advantages of surface modified nanocellulose is also discussed.
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    Iguchi, M.; Yamanaka, S.; Budhiono, A. Bacterial cellulose─a masterpiece of nature’s arts. J. Mater. Sci. 2000, 35, 261– 270,  DOI: 10.1023/a:1004775229149
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    Bacterial cellulose - a masterpiece of Nature's arts
    Iguchi, M.; Yamanaka, S.; Budhiono, A.
    Journal of Materials Science (2000), 35 (2), 261-270CODEN: JMTSAS; ISSN:0022-2461. (Kluwer Academic Publishers)
    A review with 41 refs. Ever since its remarkable mech. properties were found fifteen years ago, interest has grown in bacterial cellulose for which the use had been more or less limited to the manuf. of nata-de-coco, an indigenous food of Southeast Asia. This paper reviews the progress of relevant studies, including the prodn. of cellulose by bacteria, the formation of microfibrils and gel layer, the properties of gel and processed sheets, and some aspects of applications.
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    Fleury, B.; Abraham, E.; De La Cruz, J. A.; Chandrasekar, V. S.; Senyuk, B.; Liu, Q.; Cherpak, V.; Park, S.; ten Hove, J. B.; Smalyukh, I. I. Aerogel from Sustainably Grown Bacterial Cellulose Pellicles as a Thermally Insulative Film for Building Envelopes. ACS Appl. Mater. Interfaces 2020, 12, 34115– 34121,  DOI: 10.1021/acsami.0c08879
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    Aerogel from Sustainably Grown Bacterial Cellulose Pellicles as a Thermally Insulative Film for Building Envelopes
    Fleury, Blaise; Abraham, Eldho; De La Cruz, Joshua A.; Chandrasekar, Varun S.; Senyuk, Bohdan; Liu, Qingkun; Cherpak, Vladyslav; Park, Sungoh; ten Hove, Jan Bart; Smalyukh, Ivan I.
    ACS Applied Materials & Interfaces (2020), 12 (30), 34115-34121CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
    Improving building energy performance requires the development of new highly insulative materials. An affordable retrofitting soln. comprising a thin film could improve the resistance to heat flow in both residential and com. buildings and reduce overall energy consumption. Here, we propose cellulose aerogel films formed from pellicles produced by the bacteria Gluconacetobacter hansenii as insulation materials. We studied the impact of the d. and nanostructure on the aerogels' thermal properties. A thermal cond. as low as 13 mW/(K·m) was measured for native pellicle-based aerogels that were dried as-is with minimal post-treatment. The use of waste from the beer brewing industry as a soln. to grow the pellicle maintained the cellulose yield obtained with std. Hestrin-Schramm media, making our product more affordable and sustainable. In the future, our work can be extended through further diversification of food wastes as the substrate sources, facilitating higher potential prodn. and larger applications.
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    Chen, Y.; Zhang, L.; Yang, Y.; Pang, B.; Xu, W.; Duan, G.; Jiang, S.; Zhang, K. Recent Progress on Nanocellulose Aerogels: Preparation, Modification, Composite Fabrication, Applications. Adv. Mater. 2021, 33, 2005569,  DOI: 10.1002/adma.202005569
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    Recent Progress on Nanocellulose Aerogels: Preparation, Modification, Composite Fabrication, Applications
    Chen, Yiming; Zhang, Lin; Yang, Yang; Pang, Bo; Xu, Wenhui; Duan, Gaigai; Jiang, Shaohua; Zhang, Kai
    Advanced Materials (Weinheim, Germany) (2021), 33 (11), 2005569CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)
    A review. The rapid development of modern industry and excessive consumption of petroleum-based polymers have triggered a double crisis presenting a shortage of nonrenewable resources and environmental pollution. However, this has provided an opportunity to stimulate researchers to harness native biobased materials for novel advanced materials and applications. Nanocellulose-based aerogels, using abundant and sustainable cellulose as raw material, present a third-generation of aerogels that combine traditional aerogels with high porosity and large sp. surface area, as well as the excellent properties of cellulose itself. Currently, nanocellulose aerogels provide a highly attention-catching platform for a wide range of functional applications in various fields, e.g., adsorption, sepn., energy storage, thermal insulation, electromagnetic interference shielding, and biomedical applications. Here, the prepn. methods, modification strategies, composite fabrications, and further applications of nanocellulose aerogels are summarized, with addnl. discussions regarding the prospects and potential challenges in future development.
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    Huang, Y.; Huang, X.; Ma, M.; Hu, C.; Seidi, F.; Yin, S.; Xiao, H. Recent advances on the bacterial cellulose-derived carbon aerogels. J. Mater. Chem. C 2021, 9, 818– 828,  DOI: 10.1039/d0tc05433j
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    Recent advances on the bacterial cellulose-derived carbon aerogels
    Huang, Yang; Huang, Xiangzhou; Ma, Mengtao; Hu, Chenyao; Seidi, Farzad; Yin, Sha; Xiao, Huining
    Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2021), 9 (3), 818-828CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
    A review. Bacterial cellulose (BC), sustainable biomass, has long been envisioned as a fantastic biomass material since it was discovered by Brown in 1886. BC cultivated in static medium appears as a never-dried hydrogel, wherein numerous nanofibers are highly interconnected, building into a three-dimensional (3D) architecture. Although BC has achieved great success in the area of biol. medicine, the electronic inertness and susceptible bio-invasion restrict its further applications demanding electronic migration and durability. Carbonization has been employed to endow BC with superior cond. and chem. tolerance without destroying the 3D architecture. Moreover, carbonized BC (CBC) exhibits exceptional properties such as ultralightweight, high surface area, good volumetric resilience, and superhydrophobicity, which are necessary for electrochem. energy, microwave attenuation, and selective absorption. The industrial prodn. of BC facilitates the massive fabrication of high value-added CBC with low-cost precursors. This review summarizes the latest developments on the CBC-based functional materials, including state-of-the-art design concepts and synthetic strategies. Our prospects on the major obstacles in the approach of further exploitation of CBC, as well as the promising avenues in front of these issues are proposed in this review.
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    Pham, T. T.; Tran, T. T. A. Evaluation of the crystallinity of bacterial cellulose produced from pineapple waste solution by using acetobacter xylinum. ASEAN Eng. J. 2023, 13, 81– 91,  DOI: 10.11113/aej.v13.18868
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    Feng, J.; Nguyen, S. T.; Fan, Z.; Duong, H. M. Advanced fabrication and oil absorption properties of super-hydrophobic recycled cellulose aerogels. Chem. Eng. J. 2015, 270, 168– 175,  DOI: 10.1016/j.cej.2015.02.034
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    Advanced fabrication and oil absorption properties of super-hydrophobic recycled cellulose aerogels
    Feng, Jingduo; Nguyen, Son T.; Fan, Zeng; Duong, Hai M.
    Chemical Engineering Journal (Amsterdam, Netherlands) (2015), 270 (), 168-175CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
    A facile and cost-effective synthesis method of biocompatible cellulose aerogels using recycled cellulose fibers of paper waste and Kymene crosslinker is successfully developed for the first time. After coated with methyltrimethoxysilane (MTMS) via chem. vapor deposition, the recycled cellulose aerogels yields very stable super-hydrophobicity for over five months and excellent oil absorption capacities of up to 95 g g-1 with the 0.25 wt.% cellulose aerogel. Effects of different cellulose fiber concns., different ratios of the cellulose and Kymene crosslinker compn., ambient temps. and pH values of the environment on the oil absorption behavior of the cellulose aerogels are also quantified comprehensively. The exptl. results show the cellulose aerogels yield the max. absorption capacity at 50 °C. Compared to the pseudo first-order model, the pseudo second-order model is more validated for the oil absorption kinetics study. The recycled cellulose aerogels are promising for replacing earth-unfriendly polymer-based oil sorbents due to their high oil absorption capacities.
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    Eichhorn, S. J.; Sampson, W. W. Relationships between specific surface area and pore size in electrospun polymer fibre networks. J. R. Soc., Interface 2010, 7, 641– 649,  DOI: 10.1098/rsif.2009.0374
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    Relationships between specific surface area and pore size in electrospun polymer fibre networks
    Eichhorn, S. J.; Sampson, W. W.
    Journal of the Royal Society, Interface (2010), 7 (45), 641-649CODEN: JRSICU; ISSN:1742-5689. (Royal Society)
    From consideration of the extent of contact between fibers in electrospun polymer networks, we provide theory relating the sp. surface area of the network to the characteristic dimensions of interfiber voids. We show that these properties are strongly influenced by the cross-sectional morphologies of fibers. Whereas porosity has a strong influence on pore dimensions, in the range of porosities typically obtained in real networks, its influence on sp. surface area is weak. By considering ref. geometries of collapsed ribbons and fibers with circular cross sections, we demonstrate that at a given network porosity, fiber parameters that increase the sp. surface area reduce the characteristic dimensions of voids. The implications of the theory, mainly in the context of cell proliferation on electrospun polymer scaffolds, are discussed; the theory has relevance also to future applications of these materials in composites.
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    Cervin, N. T.; Aulin, C.; Larsson, P. T.; Wågberg, L. Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids. Cellulose 2012, 19, 401– 410,  DOI: 10.1007/s10570-011-9629-5
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    Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids
    Cervin, Nicholas Tchang; Aulin, Christian; Larsson, Per Tomas; Waagberg, Lars
    Cellulose (Dordrecht, Netherlands) (2012), 19 (2), 401-410CODEN: CELLE8; ISSN:0969-0239. (Springer)
    A novel type of sponge-like material for the sepn. of mixed oil and water liqs. has been prepd. by the vapor deposition of hydrophobic silanes on ultra-porous nanocellulose aerogels. To achieve this, a highly porous (>99%) nanocellulose aerogel with high structural flexibility and robustness is first formed by freeze-drying an aq. dispersion of the nanocellulose. The d., pore size distribution and wetting properties of the aerogel can be tuned by selecting the concn. of the nanocellulose dispersion before freeze-drying. The hydrophobic light- wt. aerogels are almost instantly filled with the oil phase when selectively absorbing oil from water, with a capacity to absorb up to 45 times their own wt. in oil. The oil can also be drained from the aerogel and the aerogel can then be reused for a second absorption cycle.
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    Revellame, E. D.; Fortela, D. L.; Sharp, W.; Hernandez, R.; Zappi, M. E. Adsorption kinetic modeling using pseudo-first order and pseudo-second order rate laws: A review. Clean. Eng. and Technol. 2020, 1, 100032,  DOI: 10.1016/j.clet.2020.100032
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    Kalam, S.; Abu-Khamsin, S. A.; Kamal, M. S.; Patil, S. Surfactant Adsorption Isotherms: A Review. ACS Omega 2021, 6, 32342– 32348,  DOI: 10.1021/acsomega.1c04661
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    Surfactant Adsorption Isotherms: A Review
    Kalam, Shams; Abu-Khamsin, Sidqi A.; Kamal, Muhammad Shahzad; Patil, Shirish
    ACS Omega (2021), 6 (48), 32342-32348CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    A review. The need to minimize surfactant adsorption on rock surfaces has been a challenge for surfactant-based, chem.-enhanced oil recovery (cEOR) techniques. Modeling of adsorption exptl. data is very useful in estg. the extent of adsorption and, hence, optimizing the process. This paper presents a mini-review of surfactant adsorption isotherms, focusing on theories of adsorption and the most frequently used adsorption isotherm models. Two-step and four-region adsorption theories are well-known, with the former representing adsorption in two steps, while the latter distinguishes four regions in the adsorption isotherm. Langmuir and Freundlich are two-parameter adsorption isotherms that are widely used in cEOR studies. The Langmuir isotherm is applied to monolayer adsorption on homogeneous sites, whereas the Freundlich isotherm suites are applied to multilayer adsorption on heterogeneous sites. Some more complex adsorption isotherms are also discussed in this paper, such as Redlich-Peterson and Sips isotherms, both involve three parameters. This paper will help select and apply a suitable adsorption isotherm to exptl. data.
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    Mullet, M.; Fievet, P.; Szymczyk, A.; Foissy, A.; Reggiani, J. C.; Pagetti, J. A simple and accurate determination of the point of zero charge of ceramic membranes. Desalination 1999, 121, 41– 48,  DOI: 10.1016/s0011-9164(99)00006-5
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    A simple and accurate determination of the point of zero charge of ceramic membranes
    Mullet, M.; Fievet, P.; Szymczyk, A.; Foissy, A.; Reggiani, J.-C.; Pagetti, J.
    Desalination (1999), 121 (1), 41-48CODEN: DSLNAH; ISSN:0011-9164. (Elsevier Science B.V.)
    A simple, accurate detn. of the point of zero charge (PZC) of a ceramic membrane is reported, based on pH variation measurements on adding an amphoteric oxide in a soln. of a given pH. Up to now, this method was effective for studying powder dispersions; in this work it was extended to ceramic membranes. An exptl. set-up that allows the performance of pH measurements on a soln. continuously circulating through the membrane is discussed. It verified that the PZC, detd. in presence of an indifferent electrolyte, is the same as the isoelec. point (or PZC) detd. with std. electrokinetic methods. The shift in the PZC towards a higher and lower pH, in presence of Na2SO4 and CaCl2 solns., resp., confirmed the specific adsorption of SO42- and Ca2+ ions and validated the method used. This method was compared with the known salt addn. method, conducted on the crushed membrane. This led to a different PZC value, demonstrating the importance of performing measurements directly on membranes themselves. Another interesting aspect in the method presented is that it permits direct assessment of the abs. value of the surface charge d. of the membrane. Results obtained were in good agreement with data reported in the literature on mineral oxides.
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    Abral, H.; Lawrensius, V.; Handayani, D.; Sugiarti, E. Preparation of nano-sized particles from bacterial cellulose using ultrasonication and their characterization. Carbohydr. Polym. 2018, 191, 161– 167,  DOI: 10.1016/j.carbpol.2018.03.026
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    Preparation of nano-sized particles from bacterial cellulose using ultrasonication and their characterization
    Abral, Hairul; Lawrensius, Vincent; Handayani, Dian; Sugiarti, Eni
    Carbohydrate Polymers (2018), 191 (), 161-167CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
    As more applications for nano-sized natural particles are discovered, simple, environmentally friendly ways to produce these particles become more important. This work preps. and characterizes nano-size bacterial cellulose particles using ultrasonication. Pellicle from nata de coco contg. nanofibers was broken up in an elec. blender, then sonicated using an ultrasonic probe at 20kHz and 3W/mL for 30, 60 and 90 min. Transmission electron microscope observations indicate the particles become nano-sized after 60 min ultrasound. The max. decompn. temp. before sonication was 373°, decreased to 357° after 60 min ultrasonication. Moisture absorption of the 90 min sonicated particles film is 60% slower compared to non-sonicated particles. After ultrasonication, the crystallinity index of the cellulose decreases. The functional groups of non-sonicated and sonicated cellulose remain the same. This study promotes a potential method of fabrication of nano-sized particles from pure bacterial cellulose.
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    Li, Z.; Zhong, L.; Zhang, T.; Qiu, F.; Yue, X.; Yang, D. Sustainable, Flexible, and Superhydrophobic Functionalized Cellulose Aerogel for Selective and Versatile Oil/Water Separation. ACS Sustain. Chem. Eng. 2019, 7, 9984– 9994,  DOI: 10.1021/acssuschemeng.9b01122
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    Sustainable, Flexible, and Superhydrophobic Functionalized Cellulose Aerogel for Selective and Versatile Oil/Water Separation
    Li, Zhangdi; Zhong, Li; Zhang, Tao; Qiu, Fengxian; Yue, Xuejie; Yang, Dongya
    ACS Sustainable Chemistry & Engineering (2019), 7 (11), 9984-9994CODEN: ASCECG; ISSN:2168-0485. (American Chemical Society)
    Aerogels, as ultralight three-dimensional (3D) highly porous materials, show great superiority in oil and org. pollutant cleanup. Notably, biomass aerogels have also attracted wide interest due to the advantages of huge reserves, low cost, renewability, biodegrdn., and nontoxicity to the environment. Herein, a sustainable, flexible, and superhydrophobic functionalized cellulose aerogel, copper nanoparticles-coated cellulose aerogel (Cu/CEA), is reported. The hydrophobic Cu/CEA was simply fabricated by one-step depositing Cu nanoparticles coating on the cellulose fibers extd. from renewable natural sisal in liq. phase followed by freeze-drying. The hydrophobic functionalization approach is facile, cost-effective, and suitable for large-scale prodn. and environmental friendliness, without addnl. org. hydrophobic modification. The highly porous Cu/CEA as absorbent can selectively and quickly collect oily contaminant, exhibiting high oil absorption capacity and rate, and good recyclability. In addn., it can also act as a thick film to continuously and rapidly sep. oil/water mixts. including emulsions, possessing very high sepn. efficiency and flow rate. Hence, the versatile and high-performance functionalized cellulose aerogel possesses a promising practical application in oily wastewater treatment and pollution remediation.
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  38. 38
    Mohamed, M. A.; Abd Mutalib, M.; Mohd Hir, Z. A.; M Zain, M.; Mohamad, A. B.; Jeffery Minggu, L.; Awang, N. A.; Salleh, W.; Salleh, W. N. An overview on cellulose-based material in tailoring bio-hybrid nanostructured photocatalysts for water treatment and renewable energy applications. Int. J. Biol. Macromol. 2017, 103, 1232– 1256,  DOI: 10.1016/j.ijbiomac.2017.05.181
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    An overview on cellulose-based material in tailoring bio-hybrid nanostructured photocatalysts for water treatment and renewable energy applications
    Mohamed, Mohamad Azuwa; Abd Mutalib, Muhazri; Mohd. Hir, Zul Adlan; Zain, M. F. M.; Mohamad, Abu Bakar; Minggu, Lorna Jeffery; Awang, Nor Asikin; Salleh, W. N. W.
    International Journal of Biological Macromolecules (2017), 103 (), 1232-1256CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    A review. A combination between the nanostructured photocatalyst and cellulose-based materials promotes a new functionality of cellulose towards the development of new bio-hybrid materials for various applications esp. in water treatment and renewable energy. The excellent compatibility and assocn. between nanostructured photocatalyst and cellulose-based materials was induced by bio-combability and high hydrophilicity of the cellulose components. The electron rich hydroxyl group of celluloses helps to promote superior interaction with photocatalyst. The formation of bio-hybrid nanostructured are attaining huge interest nowadays due to the synergistic properties of individual cellulose-based material and photocatalyst nanoparticles. Therefore, in this review we introduce some cellulose-based material and discusses its compatibility with nanostructured photocatalyst in terms of phys. and chem. properties. In addn., we gather information and evidence on the fabrication techniques of cellulose-based hybrid nanostructured photocatalyst and its recent application in the field of water treatment and renewable energy.
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    Mohamad, S.; Abdullah, L. C.; Jamari, S. S.; Al Edrus, S. S. O.; Aung, M. M.; Mohamad, S. F. S. Influence of drying method on the crystal structure and thermal property of oil palm frond juice-based bacterial cellulose. J. Mater. Sci. 2022, 57, 1462– 1473,  DOI: 10.1007/s10853-021-06685-5
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    Influence of drying method on the crystal structure and thermal property of oil palm frond juice-based bacterial cellulose
    Mohamad, Shahril; Abdullah, Luqman Chuah; Jamari, Saidatul Shima; Al Edrus, Syeed Saifulazry Osman; Aung, Min Min; Mohamad, Sharifah Fathiyah Sy
    Journal of Materials Science (2022), 57 (2), 1462-1473CODEN: JMTSAS; ISSN:0022-2461. (Springer)
    Dehydration of wet bacterial cellulose (BC) mainly focuses on the phys. characteristic or mech. strength, but its polymorph crystal structure and thermal properties were rarely discussed. Herein, this study utilizes the drying method of hot-pressed and freeze-dried to the wet BC to elucidate the BC polymorph crystal structure in correlation with the BC crystallinity and thermal properties. The results indicate that dehydration of BC using hot-pressed (BC-HP) method reduced the cellulose Iα allomorph fraction by ± 5.0%, increased the crystallinity by ± 5.0%, but lower in thermal stability compared to freeze-dried (BC-FD) method. Addnl., BC-HP shows an exothermic reaction of melting at lower enthalpy value which is contradict to BC-FD and plant cellulose that presented an endothermic reaction with higher enthalpy values. Thus, investigation on BC polymorph crystal structure and thermal properties may offer an important role to regulate the desired characteristic of the dried BC.
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    Illa, M. P.; Sharma, C. S.; Khandelwal, M. Tuning the physiochemical properties of bacterial cellulose: effect of drying conditions. J. Mater. Sci. 2019, 54, 12024– 12035,  DOI: 10.1007/s10853-019-03737-9
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    Tuning the physiochemical properties of bacterial cellulose: effect of drying conditions
    Illa, Mani Pujitha; Sharma, Chandra S.; Khandelwal, Mudrika
    Journal of Materials Science (2019), 54 (18), 12024-12035CODEN: JMTSAS; ISSN:0022-2461. (Springer)
    Bacteria have an ability to produce cellulose in pure form without any impurities such as hemicellulose and lignin, unlike plant cellulose. Bacterial cellulose as-produced with 3-D interwoven nanofibrous network is superior to plant cellulose in terms of mech. properties, porosity, crystallinity, water holding capacity, and sustainability. In its natural form, bacterial cellulose is in the form of a hydrogel, which implies high porosity and holding capacity, however, to use it for different applications, water needs to be removed. The phys. properties of bacterial cellulose such as morphol., porosity, and mech. strength are vastly affected by the drying method employed. This paper presents a case study in which we produced bacterial cellulose using two different strains, followed by systematically studying the effect of drying (oven and freeze drying) on physiochem., morphol., and structural properties of as-produced bacterial cellulose using Fourier transform IR spectroscopy, X-ray diffraction, field emission SEM, BET surface area, and tensile testing. Oven-dried bacterial cellulose showed higher crystallinity, reduced fiber diam., and narrow size distribution and higher mech. properties as compared to freeze-dried bacterial cellulose. Understanding so developed in this work may allow us to simply tune the bacterial cellulose properties for a given application.
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    Ul-Islam, M.; Khattak, W. A.; Kang, M.; Kim, S. M.; Khan, T.; Park, J. K. Effect of post-synthetic processing conditions on structural variations and applications of bacterial cellulose. Cellulose 2013, 20, 253– 263,  DOI: 10.1007/s10570-012-9799-9
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    Effect of post-synthetic processing conditions on structural variations and applications of bacterial cellulose
    Ul-Islam, Mazhar; Khattak, Waleed Ahmad; Kang, Minkyung; Kim, Sang Min; Khan, Taous; Park, Joong Kon
    Cellulose (Dordrecht, Netherlands) (2013), 20 (1), 253-263CODEN: CELLE8; ISSN:0969-0239. (Springer)
    Physicochem. properties of materials can be amended by altering their phys. structure through different processing conditions. The present study was conducted to investigate the post-synthesis structural variations and physico-mech. properties of bacterial cellulose (BC) sheets prepd. using different drying methods. Wet BC sheets of the same origin were freeze dried (BC-FD), dried at room temp. (25 °C) (BC-DRT), and dried at elevated temp. (50 °C) (BC-DHT). FE-SEM micrographs revealed that BC-DRT and BC-DHT had a more tightly packed and compact structure than the loosely held fibrils of BC-FD. XRD anal. revealed the relative crystallinity of the BC sample to be 64.60, 59.16, and 47.20 % for BC-DHT, BC-DRT and BC-FD, resp. The water holding capacity (WHC) of the BC-FD was higher than that of the other two samples. Four consecutive drying and rewetting cycles demonstrated that the WHC of all samples decreased with each cycle. The WHC of BC-DRT and BC-DHT was reduced to almost 0 after the first drying cycle, but the BC-FD samples were able to regain some of their WHC. The tensile strength and elongation modulus were in the order of BC-DHT > BC-DRT > BC-FD. Overall, the results of this study revealed that the post-synthetic processing conditions had a strong effect on the structure and physico-mech. properties of BC.
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    Zhang, C. J.; Wang, L.; Zhao, J. C.; Zhu, P. Effect of Drying Methods on Structure and Mechanical Properties of Bacterial Cellulose Films. Adv. Mater. Res. 2011, 239–242, 2667– 2670,  DOI: 10.4028/www.scientific.net/amr.239-242.2667
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    Effect of drying methods on structure and mechanical properties of bacterial cellulose films
    Zhang, Chuanjie; Wang, Liu; Zhao, Jinchao; Zhu, Ping
    Advanced Materials Research (Durnten-Zurich, Switzerland) (2011), 239-242 (Pt. 4, Advanced Materials), 2667-2670CODEN: AMREFI; ISSN:1022-6680. (Trans Tech Publications Ltd.)
    Bacterial cellulose (BC) gelatinous films prepd. in stationary culture were dried by three different drying methods: hot air drying, vacuum drying and vacuum freezing drying. The structure of dried bacterial cellulose films was characterized using SEM, IR spectroscopy and X-ray diffraction (XRD), and mech. properties were tested. The results showed that the surface of films prepd. by hot air drying were uniform and dense, cavities and cracks configurations existed in vacuum dried films, and layer and porous structures were obsd. in vacuum freezing dried films. FTIR spectra and X-ray pattern confirmed that vacuum freezing drying reduced the strength of hydrogen bonds between cellulose macromols. and the degree of crystallinity of BC films but had little influence on the crystal structure. For those reasons, mech. properties of BC films prepd. by vacuum freezing drying were lower than that of those films by other methods.
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    Zimmermann, M. V. G.; Borsoi, C.; Lavoratti, A.; Zanini, M.; Zattera, A. J.; Santana, R. M. C. Drying techniques applied to cellulose nanofibers. J. Reinf. Plast. Compos. 2016, 35, 682– 697,  DOI: 10.1177/0731684415626286
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    Drying techniques applied to cellulose nanofibers
    Zimmermann, Matheus V. G.; Borsoi, Cleide; Lavoratti, Alessandra; Zanini, Marcia; Zattera, Ademir J.; Santana, Ruth M. C.
    Journal of Reinforced Plastics and Composites (2016), 35 (8), 682-697CODEN: JRPCDW; ISSN:0731-6844. (Sage Publications Ltd.)
    A review. Nanotechnol. applied to cellulosic fibers has quickly become an interdisciplinary field with great interest in the application as reinforcement in polymer composites, mainly due to the abundance of these raw materials, and to their mech. properties and multifunctionality. However, one of the crit. points to obtain individualized cellulose nanofibers is the drying technique (dehydration), since most of the nanofiber processes are performed in the liq. phase. According to the methodol. applied to the cellulose water dehydration process, various morphologies and properties can be obtained in the cellulose fibers. This review study aims to discuss the main processes used to obtain nanocellulose (chem. and mech.) and the drying techniques applied to nanocellulose structures, such as conventional oven drying, freeze drying (lyophilization), supercrit. extn., and spray drying.
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    Liebner, F.; Potthast, A.; Rosenau, T.; Haimer, E.; Wendland, M. Cellulose aerogels: Highly porous, ultra-lightweight materials. Holzforschung 2008, 62, 129– 135,  DOI: 10.1515/hf.2008.051
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    Cellulose aerogels: highly porous, ultra-lightweight materials
    Liebner, Falk; Potthast, Antje; Rosenau, Thomas; Haimer, Emmerich; Wendland, Martin
    Holzforschung (2008), 62 (2), 129-135CODEN: HOLZAZ; ISSN:0018-3830. (Walter de Gruyter GmbH & Co. KG)
    Cellulosic aerogels are intriguing new materials produced by supercrit. drying of regenerated cellulose obtained by solvent exchange of solid Lyocell moldings. From N-methylmorpholine-N-oxide (NMMO) solns. with cellulose contents between 1 and 12%, dimensionally stable cellulose bodies are produced, in which the soln. structure of the cellulose is largely preserved and transferred into the solid state, the material having densities down to 0.05 g cm-3 and surface areas of up to 280 m2 g-1. In this study, several aspects of cellulosic aerogel prodn. are communicated: the stabilization of the cellulose solns. against degrdn. reactions by agents suitable for later extn. and drying, a reliable extn. and drying procedure by supercrit. carbon dioxide, the advantages of DMSO/NMMO in this procedure as a solvent/non-solvent pair, and some data on the phys. properties of the materials.
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    Liebner, F.; Haimer, E.; Potthast, A.; Loidl, D.; Tschegg, S.; Neouze, M.-A.; Wendland, M.; Rosenau, T. Cellulosic aerogels as ultra-lightweight materials. Part 2: Synthesis and properties 2nd ICC 2007, Tokyo, Japan, October 25–29, 2007. Holzforschung 2009, 63, 3– 11,  DOI: 10.1515/hf.2009.002
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    Cellulosic aerogels as ultra-lightweight materials. Part 2: synthesis and properties
    Liebner, Falk; Haimer, Emmerich; Potthast, Antje; Loidl, Dieter; Tschegg, Stefanie; Neouze, Marie-Alexandra; Wendland, Martin; Rosenau, Thomas
    Holzforschung (2009), 63 (1), 3-11CODEN: HOLZAZ; ISSN:0018-3830. (Walter de Gruyter GmbH & Co. KG)
    Ultra-lightwt. cellulose aerogels can be obtained in three steps: (1) prepn. of a cellulose soln. in molten N-methylmorpholine-N-oxide monohydrate (NMMO·H2O) at 110-120°C and casting of the viscous mass into molds; (2) extn. of the solidified castings with ethanol to initiate cellulose aggregation and to remove NMMO·H2O so that the fragile, fine-porous texture of cellulose II is largely retained; and (3) drying of the lyogel using supercrit. carbon dioxide (scCO2). According to this approach, cellulosic aerogels were prepd. from eight com. cellulosic materials and pulps and analyzed for selected chem., physicochem. and mech. parameters. The results reveal that all aerogels obtained from 3% cellulose contg. NMMO·H2O melts had a largely uniform mesoporous structure with an av. pore size of ∼9-12 nm, surface area of 190-310 m2 g-1, and specific d. of 0.046-0.069 g cm-3, but rather low mech. stability expressed as compressive yield strain of 2.9-5.5%. All samples showed viscoelastic behavior, with Young's modulus ranging from ∼5 to 10 N mm-2. Doubling the cellulose content in the NMMO·H2O melt from 3% to 6% increased Young's modulus by one order of magnitude. Shrinkage of the fragile cellulose bodies during scCO2 drying was still considerable and is subject to further investigations. Influencing parameters such as scCO2 pressure, cellulose content, regenerating solvent and the no. of regenerating baths were optimized.
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    Liebner, F.; Haimer, E.; Wendland, M.; Neouze, M. A.; Schlufter, K.; Miethe, P.; Heinze, T.; Potthast, A.; Rosenau, T. Aerogels from unaltered bacterial cellulose: application of scCO2 drying for the preparation of shaped, ultra-lightweight cellulosic aerogels. Macromol. Biosci. 2010, 10, 349– 352,  DOI: 10.1002/mabi.200900371
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    Aerogels from Unaltered Bacterial Cellulose: application of scCO2 Drying for the Preparation of Shaped, Ultra-Lightweight Cellulosic Aerogels
    Liebner, Falk; Haimer, Emmerich; Wendland, Martin; Neouze, Marie-Alexandra; Schlufter, Kerstin; Miethe, Peter; Heinze, Thomas; Potthast, Antje; Rosenau, Thomas
    Macromolecular Bioscience (2010), 10 (4), 349-352CODEN: MBAIBU; ISSN:1616-5187. (Wiley-VCH Verlag GmbH & Co. KGaA)
    Bacterial cellulose produced by the gram-neg. bacterium Gluconacetobacter xylinum was found to be an excellent native starting material for prepg. shaped ultra-lightwt. cellulose aerogels. The procedure comprises thorough washing and sterilization of the aquogel, quant. solvent exchange and subsequent drying with supercrit. carbon dioxide at 40° and 100 bar. The av. d. of the obtained dry cellulose aerogels is only about 8 mg/cm-3 which is comparable to the most lightwt. silica aerogels and distinctly lower than all values for cellulosic aerogels obtained from plant cellulose so far. SEM, ESEM, and nitrogen adsorption expts. at 77 K reveal an open-porous network structure that consists of a comparatively high percentage of large mesopores and smaller macropores.
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    Chang, S. S.; Clair, B.; Ruelle, J.; Beauchene, J.; Di Renzo, F.; Quignard, F.; Zhao, G. J.; Yamamoto, H.; Gril, J. Mesoporosity as a new parameter for understanding tension stress generation in trees. J. Exp. Bot. 2009, 60, 3023– 3030,  DOI: 10.1093/jxb/erp133
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    Mesoporosity as a new parameter for understanding tension stress generation in trees
    Chang, Shan-Shan; Clair, Bruno; Ruelle, Julien; Beauchene, Jacques; Di Renzo, Francesco; Quignard, Francoise; Zhao, Guang-Jie; Yamamoto, Hiroyuki; Gril, Joseph
    Journal of Experimental Botany (2009), 60 (11), 3023-3030CODEN: JEBOA6; ISSN:0022-0957. (Oxford University Press)
    The mechanism for tree orientation in angiosperms is based on the prodn. of high tensile stress on the upper side of the inclined axis. In many species, the stress level is strongly related to the presence of a peculiar layer, called the G-layer, in the fiber cell wall. The structure of the G-layer has recently been described as a hydrogel thanks to N2 adsorption-desorption isotherms of supercritically dried samples showing a high mesoporosity (pores size from 2-50 nm). This led us to revisit the concept of the G-layer that had been, until now, only described from anatomical observation. Adsorption isotherms of both normal wood and tension wood have been measured on six tropical species. Measurements show that mesoporosity is high in tension wood with a typical thick G-layer while it is much less with a thinner G-layer, sometimes no more than normal wood. The mesoporosity of tension wood species without a G-layer is as low as in normal wood. Not depending on the amt. of pores, the pore size distribution is always centered around 6-12 nm. These results suggest that, among species producing fibers with a G-layer, large structural differences of the G-layer exist between species.
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    Guo, J.; Catchmark, J. M. Surface area and porosity of acid hydrolyzed cellulose nanowhiskers and cellulose produced by Gluconacetobacter xylinus. Carbohydr. Polym. 2012, 87, 1026– 1037,  DOI: 10.1016/j.carbpol.2011.07.060
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    Surface area and porosity of acid hydrolyzed cellulose nanowhiskers and cellulose produced by Gluconacetobacter xylinus
    Guo, Jing; Catchmark, Jeffrey M.
    Carbohydrate Polymers (2012), 87 (2), 1026-1037CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
    The phys. parameters of cellulose such as surface area and porosity are important in the development of cellulose composites which may contain valuable additives which bind to cellulose. In this area, the use of acid hydrolyzed nano-dimensional cellulose nanowhiskers (CNWs) has attracted significant interest, yet the surface area and porosity of these materials have not been explored exptl. The objective of this work was to characterize the surface area and porosity of CNWs from different origins (plant cotton/bacterium Gluconacetobacter xylinus) and different acid treatments (H2SO4/HCl) by N2 adsorption; as well as to compare surface area and porosity of bacterial cellulose synthesized by static and agitated cultures. Our results showed that CNWs produced from H2SO4/HCl exhibited significantly increased surface area and porosity relative to starting material cotton fiber CF11. Micropores were generated in HCl hydrolyzed CNWs but not in H2SO4 hydrolyzed CNWs. Bacterial CNWs exhibited larger surface area and porosity compared to plant CNWs. Cellulose synthesized by G. xylinus ATCC 700178 from agitated cultures also exhibited less surface area and porosity than those from static cultures.
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    Horvat, G.; Pantic, M.; Knez, Z.; Novak, Z. A Brief Evaluation of Pore Structure Determination for Bioaerogels. Gels 2022, 8, 438,  DOI: 10.3390/gels8070438
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    A Brief Evaluation of Pore Structure Determination for Bioaerogels
    Horvat, Gabrijela; Pantic, Milica; Knez, Zeljko; Novak, Zoran
    Gels (2022), 8 (7), 438CODEN: GELSAZ; ISSN:2310-2861. (MDPI AG)
    A review. This review discusses the most commonly employed methods for detg. pore size and pore size distribution in bioaerogels. Aerogels are materials with high porosity and large surface areas. Most of their pores are in the range of mesopores, between 2 and 50 nm. They often have smaller or larger pores, which presents a significant challenge in detg. the exact mean pore size and pore size distribution in such materials. The precision and actual value of the pore size are of considerable importance since pore size and pore size distribution are among the main properties of aerogels and are often directly connected with the final application of those materials. However, many recently published papers discuss or present pore size as one of the essential achievements despite the misinterpretation or the wrong assignments of pore size detn. This review will help future research and publications evaluate the pore size of aerogels more precisely and discuss it correctly. The study covers methods such as gas adsorption, from which BJH and DFT models are often used, SEM, mercury porosimetry, and thermoporometry. The methods are described, and the results obtained are discussed. The following paper shows that there is still no precise method for detg. pore size distribution or mean pore size in aerogels until now. Knowing that, it is expected that this field will evolve in the future.
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    Mi, Q.-y.; Ma, S.-r.; Yu, J.; He, J.-s.; Zhang, J. Flexible and Transparent Cellulose Aerogels with Uniform Nanoporous Structure by a Controlled Regeneration Process. ACS Sustain. Chem. Eng. 2016, 4, 656– 660,  DOI: 10.1021/acssuschemeng.5b01079
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    Dos Santos Silva, L.; De Oliveira Carvalho, J.; De Sousa Bezerra, R. D.; Da Silva, M. S.; Ferreira, F. J.; Osajima, J. A.; Da Silva Filho, E. C. Potential of Cellulose Functionalized with Carboxylic Acid as Biosorbent for the Removal of Cationic Dyes in Aqueous Solution. Molecules 2018, 23, 743,  DOI: 10.3390/molecules23040743
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    Lahiri, D.; Nag, M.; Dutta, B.; Dey, A.; Sarkar, T.; Pati, S.; Edinur, H. A.; Abdul Kari, Z.; Mohd Noor, N. H.; Ray, R. R. Bacterial Cellulose: Production, Characterization, and Application as Antimicrobial Agent. Int. J. Mol. Sci. 2021, 22, 12984,  DOI: 10.3390/ijms222312984
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    Bacterial Cellulose: Production, Characterization, and Application as Antimicrobial Agent
    Lahiri, Dibyajit; Nag, Moupriya; Dutta, Bandita; Dey, Ankita; Sarkar, Tanmay; Pati, Siddhartha; Edinur, Hisham Atan; Abdul Kari, Zulhisyam; Mohd Noor, Noor Haslina; Ray, Rina Rani
    International Journal of Molecular Sciences (2021), 22 (23), 12984CODEN: IJMCFK; ISSN:1422-0067. (MDPI AG)
    A review. Bacterial cellulose (BC) is recognized as a multifaceted, versatile biomaterial with abundant applications. Groups of microorganisms such as bacteria are accountable for BC synthesis through static or agitated fermn. processes in the presence of competent media. In comparison to static cultivation, agitated cultivation provides the max. yield of the BC. A pure cellulose BC can pos. interact with hydrophilic or hydrophobic biopolymers while being used in the biomedical domain. From the last two decades, the reinforcement of biopolymer-based biocomposites and its applicability with BC have increased in the research field. The harmony of hydrophobic biopolymers can be reduced due to the high moisture content of BC in comparison to hydrophilic biopolymers. Mech. properties are the important parameters not only in producing green composite but also in dealing with tissue engineering, medical implants, and biofilm. The wide requisition of BC in medical as well as industrial fields has warranted the scaling up of the prodn. of BC with added economy. This review provides a detailed overview of the prodn. and properties of BC and several parameters affecting the prodn. of BC and its biocomposites, elucidating their antimicrobial and antibiofilm efficacy with an insight to highlight their therapeutic potential.
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    Yang, H.; Yan, R.; Chen, H.; Lee, D. H.; Zheng, C. Characteristics of hemicellulose, cellulose and lignin pyrolysis. Fuel 2007, 86, 1781– 1788,  DOI: 10.1016/j.fuel.2006.12.013
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    Characteristics of hemicellulose, cellulose and lignin pyrolysis
    Yang, Haiping; Yan, Rong; Chen, Hanping; Lee, Dong Ho; Zheng, Chuguang
    Fuel (2007), 86 (12-13), 1781-1788CODEN: FUELAC; ISSN:0016-2361. (Elsevier Ltd.)
    The pyrolysis characteristics of three main components (hemicellulose, cellulose and lignin) of biomass were investigated using, resp., a thermogravimetric analyzer (TGA) with differential scanning calorimetry (DSC) detector and a pack bed. The releasing of main gas products from biomass pyrolysis in TGA was online measured using Fourier transform IR (FTIR) spectroscopy. In thermal anal., the pyrolysis of hemicellulose and cellulose occurred quickly, with the wt. loss of hemicellulose mainly happened at 220-315° and that of cellulose at 315-400°. However, lignin was more difficult to decomp., as its wt. loss happened in a wide temp. range (from 160 to 900°) and the generated solid residue was high (∼40%). From the viewpoint of energy consumption in the course of pyrolysis, cellulose behaved differently from hemicellulose and lignin; the pyrolysis of the former was endothermic while that of the latter was exothermic. The main gas products from pyrolyzing the three components were similar, including CO2, CO, CH4 and some orgs. The releasing behaviors of H2 and the total gas yield were measured using Micro-GC when pyrolyzing the three components in a packed bed. Hemicellulose had higher CO2 yield, cellulose generated higher CO yield, and lignin owned higher H2 and CH4 yield. A better understanding to the gas products releasing from biomass pyrolysis could be achieved based on this in-depth investigation on three main biomass components.
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    Eltaweil, A. S.; Elgarhy, G. S.; El-Subruiti, G. M.; Omer, A. M. Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads for efficient adsorption of cationic methylene blue dye. Int. J. Biol. Macromol. 2020, 154, 307– 318,  DOI: 10.1016/j.ijbiomac.2020.03.122
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    Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads for efficient adsorption of cationic methylene blue dye
    Eltaweil, Abdelazeem S.; Elgarhy, Gehad S.; El-Subruiti, Gehan M.; Omer, Ahmed M.
    International Journal of Biological Macromolecules (2020), 154 (), 307-318CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    An efficient composite adsorbent was fabricated based on CM-cellulose (CMC) microbeads incorporated carboxylated graphene oxide (GOCOOH) for the adsorptive removal of cationic methylene blue dye (MB). The developed CMC/GOCOOH composite microbeads were characterized by means of FTIR, TGA, SEM, XPS, BET and zeta potential anal. tools. Various parameters affecting the removal of MB dye such as the amt. of GOCOOH, initial MB concn., adsorbent dosage, pH and medium temp. were optimized using a series of batch adsorption expts. The exptl. data of the adsorption process were more fitted to Langmuir isotherm (R2 = 0.998) with a max. adsorption capacity of 180.32 mg/g and followed the pseudo-second order kinetic model. Moreover, the adsorption of MB dye onto CMC/GOCOOH composite microbeads was an exothermic process with a max. capacity at pH 10. Besides, the fabricated adsorbent exposed also better reusability for nine repetitive cycles with highly adsorption properties. The gained results imply that the CMC/GOCOOH microbeads could be potentially applied as an effective and reusable adsorbent for MB dye removal from aq. solns.
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    Chan, C. H.; Chia, C. H.; Zakaria, S.; Sajab, M. S.; Chin, S. X. Cellulose nanofibrils: a rapid adsorbent for the removal of methylene blue. RSC Adv. 2015, 5, 18204– 18212,  DOI: 10.1039/c4ra15754k
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    Cellulose nanofibrils: a rapid adsorbent for the removal of methylene blue
    Chan, Chi Hoong; Chia, Chin Hua; Zakaria, Sarani; Sajab, Mohd. Shaiful; Chin, Siew Xian
    RSC Advances (2015), 5 (24), 18204-18212CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
    Cellulose nanofibrils (CNF) were prepd. from kenaf core (KC) using acidified-chlorite bleaching method and followed by disintegration using a high speed blender. The effects of disintegration time and acid treatment on the defibrillation of holocellulose were studied. Hemicellulose was found to facilitate defibrillation, as CNF without any acid treatment was fully defibrillated after 30 min. The adsorption kinetics of CNF toward cationic dye cannot be accurately detd. due to its quick adsorption performance, in which the equil. is achieved immediately after 1 min of contact time. The effects of acid treatment on holocellulose, pH, adsorbent dosage, temp. and dye concn. were studied and optimized. Adsorption data were fitted to both Langmuir and Freundlich models where the Langmuir model was found to be the better model to describe the adsorption process. The max. adsorption capacity was found to be 122.2 mg g-1 at pH 9, 20 °C for the non-acid treated CNF. The CNF can be regenerated by desorption at low pH where as much as 70% of the dye adsorbed can be desorbed after 6 cycles of adsorption-desorption.
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    Nguyen, V. T.; Ha, L. Q.; Nguyen, T. D. L.; Ly, P. H.; Nguyen, D. M.; Hoang, D. Nanocellulose and Graphene Oxide Aerogels for Adsorption and Removal Methylene Blue from an Aqueous Environment. ACS Omega 2022, 7, 1003– 1013,  DOI: 10.1021/acsomega.1c05586
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    Nanocellulose and graphene oxide aerogels for adsorption and removal methylene blue from aqueous environment
    Nguyen, Vy T.; Ha, Lam Q.; Nguyen, Tu D. L.; Ly, Phuong H.; Nguyen, Dang Mao; Hoang, DongQuy
    ACS Omega (2022), 7 (1), 1003-1013CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    The characteristics of aerogel materials such as the low d. and large surface area enable them to adsorb large amts. of substances, so they show great potential for application in industrial wastewater treatment. Herein, using a combination of completely environmentally friendly materials such as cellulose nanofibers (CNFs) extd. from the petioles of the nipa palm tree and graphene oxide (GO) fabricated by simple solvent evapn., a composite aerogel was prepd. by a freeze-drying method. The obtained aerogel possessed a light d. of 0.0264 g/cm3 and a porosity of more than 98.2%. It was able to withstand a wt. as much as 2500 times with the max. force (1479.5 N) to break up 0.2 g of an aerogel by compression strength testing and was stable in the aquatic environment, enabling it to be reused five times with an adsorption capacity over 90%. The CNF/GO aerogel can recover higher than 85% after 30 consecutive compression recovery cycles, which is convenient for the reusability of this material in wastewater treatments. The obtained aerogel also showed a good interaction between the component phases, a high thermal stability, a 3D network structure combined with thin walls and pores with a large sp. surface area. In addn., the aerogel also exhibited a fast adsorption rate for methylene blue (MB) adsorption, a type of waste from the textile industry that pollutes water sources, and it can adsorb more than 99% MB in water in less than 20 min. The excellent adsorption of MB onto the CNF/GO aerogel was driven by electrostatic interactions, which agreed with the pseudo-second-order kinetic model with a correlation coeff. R2 = 0.9978. The initial results show that the CNF/GO aerogel is a highly durable "green" light material that might be applied in the treatment of domestic org. waste water and is completely recoverable and reusable.
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    Huang, J.; Yan, Z. Adsorption Mechanism of Oil by Resilient Graphene Aerogels from Oil–Water Emulsion. Langmuir 2018, 34, 1890– 1898,  DOI: 10.1021/acs.langmuir.7b03866
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    Adsorption Mechanism of Oil by Resilient Graphene Aerogels from Oil-Water Emulsion
    Huang, Jiankun; Yan, Zifeng
    Langmuir (2018), 34 (5), 1890-1898CODEN: LANGD5; ISSN:0743-7463. (American Chemical Society)
    A facile synthesis strategy was adopted to prep. resilient graphene aerogel (GA) with properties of high emulsified oil adsorption capacities, excellent rebounding performance, oil-water selectivity, and recycling abilities. The max. adsorption capacity of GA for emulsified diesel oil was 2.5 × 104 mg g-1. The microscopic kinetic and thermodn. mutual reaction models of diesel oil emulsion adsorption onto GA were investigated to describe the adsorption mechanism. The emulsified diesel oil was able to be sepd. efficiently from the oil-water emulsion by GA because of their high oil selectivity. Interestingly, both kinetics and thermodn. expts. show that emulsified oil adsorption on GA is a phys. adsorption and spontaneous process. Besides, GA can be reused with prominent repeatability for at least 10 cycles, demonstrating feasibility in practical applications of GA-based oily water treatment.
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    Luo, M.; Wang, M.; Pang, H.; Zhang, R.; Huang, J.; Liang, K.; Chen, P.; Sun, P.; Kong, B. Super-assembled highly compressible and flexible cellulose aerogels for methylene blue removal from water. Chin. Chem. Lett. 2021, 32, 2091– 2096,  DOI: 10.1016/j.cclet.2021.03.024
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    Super-assembled highly compressible and flexible cellulose aerogels for methylene blue removal from water
    Luo, Mingfu; Wang, Meng; Pang, Huaipeng; Zhang, Runhao; Huang, Jing; Liang, Kang; Chen, Pu; Sun, Peipei; Kong, Biao
    Chinese Chemical Letters (2021), 32 (6), 2091-2096CODEN: CCLEE7; ISSN:1001-8417. (Elsevier B.V.)
    Phys. adsorption is a common method to solve the contamination of methylene blue in dyeing wastewater. As a kind of adsorption material, cellulose aerogels with high porosity and surface areas have great potential application in methylene blue removal. However, the week hydrogen bonding between cellulose nanofibers making the cellulose aerogels with the poor mech. properties and can be easily destroyed during adsorption. Hence, the prepn. of cellulose aerogels with high mech. strength is still a great challenge. Here, we report a robust super-assembly strategy to fabricate cellulose aerogels by combining cellulose nanofibers with PVA and M-K10. The resulting cellulose aerogels not only has a robust chem. cross-linked network, but also has strong H-bonds, which greatly enhance the mech. properties. The resulting cellulose aerogels possess a low d. of 19.32 mg/cm3. Furthermore, the cellulose aerogel shows 93% shape recovery under 60% strain (9.5 kPa under 60% strain) after 100 cycles, showing excellent mech. property. The adsorption capacity of cellulose aerogel to methylene blue soln. of 20 mg/L is 2.28 mg/g and the adsorption kinetics and adsorption isotherms have also been studied. Pseudo-second-order kinetic model and Freundlich isotherm model are more acceptable for indicating the adsorption process of methylene blue on the cellulose aerogel. Thus, this compressible and durable cellulose aerogel is a very prospective material for dyeing wastewater cleanup.
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    Phuong, N. T. X.; Ho, K. H.; Nguyen, C. T. X.; Dang, Y. T.; Do, N. H. N.; Le, K. A.; Do, T. C. Novel Fabrication of Renewable Aerogels from Coconut Coir Fibers for Dye Removal. Chem. Eng. Trans. 2021, 89, 31,  DOI: 10.3303/CET2189006
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    Hosseini, H.; Zirakjou, A.; McClements, D. J.; Goodarzi, V.; Chen, W.-H. Removal of methylene blue from wastewater using ternary nanocomposite aerogel systems: Carboxymethyl cellulose grafted by polyacrylic acid and decorated with graphene oxide. J. Hazard. Mater. 2022, 421, 126752,  DOI: 10.1016/j.jhazmat.2021.126752
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    Removal of methylene blue from wastewater using ternary nanocomposite aerogel systems: Carboxymethyl cellulose grafted by polyacrylic acid and decorated with graphene oxide
    Hosseini, Hadi; Zirakjou, Abbas; McClements, David Julian; Goodarzi, Vahabodin; Chen, Wei-Hsin
    Journal of Hazardous Materials (2022), 421 (), 126752CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
    In this study, environmentally-friendly nanocomposite hydrogels were fabricated. These hydrogels consisted of semi-interpenetrating networks of CM-cellulose (CMC) mols. grafted to polyacrylic acid (PAA), as an eco-friendly and non-toxic polymer with numerous carboxyl and hydroxyl functional groups, which were reinforced with different levels of graphene oxide particles (0.5, 1.5 or 3% wt). Field-emission electron scanning microscopy (FESEM) images indicated that the pore size of the nanocomposites decreased with increasing graphic oxide concn. The presence of the graphic oxide increased the storage modulus and thermal stability of the nanocomposite hydrogels. The hydrogels had an adsorption capacity of 138 mg/g of a model cationic dye pollutant (methylene blue) after 250 min. Moreover, a reusability test showed that the adsorption capacity remained at around 90% after 9 cycles. D. functional theory (DFT) simulations suggested that the adsorption of methylene blue was mainly a result of π-π bonds, hydrogen bonds, and electrostatic interactions with graphene oxide. Our results indicated that the nanocomposite hydrogels fabricated in this study may be eco-friendly, stable, efficient, and reusable adsorbents for ionic pollutants in wastewater treatment.
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    Ahmad, T.; Danish, M.; Rafatullah, M.; Ghazali, A.; Sulaiman, O.; Hashim, R.; Ibrahim, M. N. M. The use of date palm as a potential adsorbent for wastewater treatment: a review. Environ. Sci. Pollut. Res. 2012, 19, 1464– 1484,  DOI: 10.1007/s11356-011-0709-8
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    The use of date palm as a potential adsorbent for wastewater treatment: a review
    Ahmad, Tanweer; Danish, Mohammad; Rafatullah, Mohammad; Ghazali, Arniza; Sulaiman, Othman; Hashim, Rokiah; Ibrahim, Mohamad Nasir Mohamad
    Environmental Science and Pollution Research (2012), 19 (5), 1464-1484CODEN: ESPLEC; ISSN:0944-1344. (Springer)
    A review. Background In tropical countries, the palm tree is one of the most abundant and important trees. Date palm is a principal fruit grown in many regions of the world. It is abundant, locally available and effective material that could be used as an adsorbent for the removal of different pollutants from aq. soln. Review This article presents a review on the role of date palm as adsorbents in the removal of unwanted materials such as acid and basic dyes, heavy metals, and phenolic compds. Many studies on adsorption properties of various low cost adsorbent, such as agricultural waste and activated carbons based on agricultural waste have been reported in recent years. Conclusion Studies have shown that date palm-based adsorbents are the most promising adsorbents for removing unwanted materials. No previous review is available where researchers can get an overview of the adsorption capacities of date palm-based adsorbent used for the adsorption of different pollutants. This review provides the recent literature demonstrating the usefulness of date palm biomass-based adsorbents in the adsorption of various pollutants.
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  62. 62
    Nguyen, K. D.; Vo, N. T.; Le, K. T. M.; Ho, K. V.; Phan, N. T. S.; Ho, P. H.; Le, H. V. Defect-engineered metal–organic frameworks (MOF-808) towards the improved adsorptive removal of organic dyes and chromium (vi) species from water. New J. Chem. 2023, 47, 6433– 6447,  DOI: 10.1039/d2nj05693c
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    Defect-engineered metal-organic frameworks (MOF-808) towards the improved adsorptive removal of organic dyes and chromium(VI) species from water
    Nguyen, Khoa D.; Vo, Nhi T.; Le, Khanh T. M.; Ho, Khanh V.; Phan, Nam T. S.; Ho, Phuoc H.; Le, Ha V.
    New Journal of Chemistry (2023), 47 (13), 6433-6447CODEN: NJCHE5; ISSN:1144-0546. (Royal Society of Chemistry)
    Two defective Zr-based metal-org. frameworks (Zr-MOFs), MOF-808-OH and MOF-808-NH2, were synthesized by partially replacing the 1,3,5-benzenetricarboxylate building block with 5-hydroxyisophthalate and 5-aminoisophthalate, resp. The structural features of the defective materials were analyzed by powder x-ray diffraction (PXRD), SEM, N physisorption at 77 K, and TGA. Importantly, the no. of defect sites detd. via 1H NMR (1H-NMR) anal. of the digested materials was ∼7 mol% for MOF-808-OH and 3 mol% for MOF-808-NH2. The presence of the defect sites increased the no. of acidic centers on Zr-clusters originating from missing-linker nodes which accounted for a remarkable adsorption capacity towards various anionic org. dyes and Cr(VI) species. Compared to std. MOF-808, the defect-engineered ones showed significant increments by 30-60% in trapping capacity for anionic contaminants including sunset yellow, quinoline yellow, Methyl orange, and K dichromate, while they exhibited modest improvements by 5-15% in the removal of cationic dyes, malachite green and methylene blue.
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    Elsayed, I.; Schueneman, G. T.; El-Giar, E. M.; Hassan, E. B. Amino-Functionalized Cellulose Nanofiber/Lignosulfonate New Aerogel Adsorbent for the Removal of Dyes and Heavy Metals from Wastewater. Gels 2023, 9, 154,  DOI: 10.3390/gels9020154
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    Amino-Functionalized Cellulose Nanofiber/Lignosulfonate New Aerogel Adsorbent for the Removal of Dyes and Heavy Metals from Wastewater
    Elsayed, Islam; Schueneman, Gregory T.; El-Giar, Emad M.; Hassan, El Barbary
    Gels (2023), 9 (2), 154CODEN: GELSAZ; ISSN:2310-2861. (MDPI AG)
    Due to the increasingly widespread water pollutants and the high cost of treatment methods, there is a demand for new, inexpensive, renewable, and biodegradable adsorbent materials for the purifn. of wastewater contaminants. In this study, a new biocomposite aerogel (Amf-CNF/LS) was prepd. using a chem. crosslinking method between the amino-functionalized cellulose nanofibers (Amf-CNF) and lignosulfonates (LS). The phys. and chem. properties of the prepd. aerogel were investigated using several techniques including elemental anal., SEM (SEM-EDS), Fourier transform IR spectroscopy (FTIR), thermal gravimetric anal. (TGA), and N2 adsorption-desorption anal. The Amf-CNF/LS aerogel was then applied for the removal of methylene blue (MB), rhodamine B dye (RhB), and the heavy metal cadmium ion (Cd2+) from synthetic wastewater solns. The adsorption parameters controlling the adsorption process including the pH, contact time, adsorbent dosage, and adsorbate concen-tration were optimized. High adsorption kinetics and isotherms were obsd., with the adsorption isotherms of the Amf-CNF/LS aerogel fitting the Langmuir model with max. adsorption capacities of 170.94, 147.28, and 129.87 mg/g for MB, RhB, and Cd2+, resp. These results show that Amf-CNF/LS aerogel is a promising green and inexpensive adsorbent for MB, RhB, and Cd2+ removal from wastewater.
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    Salazar-Rabago, J. J.; Leyva-Ramos, R.; Rivera-Utrilla, J.; Ocampo-Perez, R.; Cerino-Cordova, F. J. Biosorption mechanism of Methylene Blue from aqueous solution onto White Pine (Pinus durangensis) sawdust: Effect of operating conditions. Sustainable Environ. Res. 2017, 27, 32– 40,  DOI: 10.1016/j.serj.2016.11.009
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    Biosorption mechanism of Methylene Blue from aqueous solution onto White Pine (Pinus durangensis) sawdust: Effect of operating conditions
    Salazar-Rabago, Jacob J.; Leyva-Ramos, Roberto; Rivera-Utrilla, Jose; Ocampo-Perez, Raul; Cerino-Cordova, Felipe J.
    Sustainable Environment Research (2017), 27 (1), 32-40CODEN: SERUBY; ISSN:2468-2039. (Elsevier B.V.)
    In this work, the biosorption mechanism of the cationic dye Methylene Blue (MB) on natural White Pine sawdust (NS) (Pinus durangensis) was investigated. Likewise, the surface charge distribution of NS was detd., and its point of zero charge was found to be 4.3. Besides, the capacity of the NS for adsorbing MB was increased 1.7, 2.0 and 4.6 times when the pH was raised from 3 to 4.25, 3 to 7 and 3 to 10, resp. This behavior was attributed to the electrostatic attraction between the neg. charged surface of NS and the cationic species MB+. The adsorption capacity increased with increased temp. because the adsorption was an endothermic process. The adsorption capacity was drastically reduced by increasing the ionic strength of the soln. corroborating with the fact that the electrostatic attractions played a crucial role in the adsorption of MB on NS. It was also shown that the MB was chemisorbed because the adsorption was not reversible. The predominant adsorption mechanisms were the electrostatic attraction and chemisorption and not ion exchange.
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    Bialik, E.; Stenqvist, B.; Fang, Y.; Östlund, Å.; Furó, I.; Lindman, B.; Lund, M.; Bernin, D. Ionization of Cellobiose in Aqueous Alkali and the Mechanism of Cellulose Dissolution. J. Phys. Chem. Lett. 2016, 7, 5044– 5048,  DOI: 10.1021/acs.jpclett.6b02346
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    Ionization of Cellobiose in Aqueous Alkali and the Mechanism of Cellulose Dissolution
    Bialik, Erik; Stenqvist, Bjoern; Fang, Yuan; Oestlund, Aasa; Furo, Istvan; Lindman, Bjoern; Lund, Mikael; Bernin, Diana
    Journal of Physical Chemistry Letters (2016), 7 (24), 5044-5048CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
    Cellulose, one of the most abundant renewable resources, is insol. in most common solvents but dissolves in aq. alkali under a narrow range of conditions. To elucidate the solubilization mechanism, we performed electrophoretic NMR on cellobiose, a subunit of cellulose, showing that cellobiose acts as an acid with two dissocn. steps at pH 12 and 13.5. Chem. shift differences between cellobiose in NaOH and NaCl were estd. using 2D NMR and compared to DFT shift differences upon deprotonation. The dissocn. steps are the deprotonation of the hemiacetal OH group and the deprotonation of one of four OH groups on the nonreducing anhydroglucose unit. MD simulations reveal that aggregation is suppressed upon charging cellulose chains in soln. Our findings strongly suggest that cellulose is to a large extent charged in concd. aq. alkali, a seemingly crucial factor for solubilization. This insight, overlooked in the current literature, is important for understanding cellulose dissoln. and for synthesis of new sustainable materials.
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    Swensson, B.; Larsson, A.; Hasani, M. Probing Interactions in Combined Hydroxide Base Solvents for Improving Dissolution of Cellulose. Polymers 2020, 12, 1310,  DOI: 10.3390/polym12061310
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    Probing interactions in combined hydroxide base solvents for improving dissolution of cellulose
    Swensson, Beatrice; Larsson, Anette; Hasani, Merima
    Polymers (Basel, Switzerland) (2020), 12 (6), 1310CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
    To further understand cellulose-solvent interactions in aq. hydroxide solns., cellulose behavior in aq. solns. of NaOH combined with tetramethylammonium hydroxide (TMAH) or benzyltrimethylammonium hydroxide (Triton B), as well as urea, was investigated. The rheol. properties of the solns. were assessed through flow sweeps at different temps., and the intermol. interactions were probed using solvatochromic dyes. The results showed that NaOH combined with TMAH had synergistic effects on cellulose dissoln. and was a better solvent for cellulose than the combination of NaOH with Triton B, in spite of the superior dissoln. ability of Triton B alone. This somewhat unexpected finding shows that the base pair needs to be selected with care. Interestingly, addn. of urea had no significant effect on the solvatochromic parameters or dissoln. capacity of solns. of Triton B but rendered improved stability of solns. contg. NaOH and/or TMAH. It seems that both urea and Triton B weaken the hydrophobic assembly effect of these solns., but urea is excluded from interacting with cellulose in the presence of Triton B. This study provides further insight into dissoln. of cellulose and the possibility of utilizing combinations of hydroxide bases to achieve improved soln. properties.
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    Wei, X.; Huang, T.; Nie, J.; Yang, J.-h.; Qi, X.-d.; Zhou, Z.-w.; Wang, Y. Bio-inspired functionalization of microcrystalline cellulose aerogel with high adsorption performance toward dyes. Carbohydr. Polym. 2018, 198, 546– 555,  DOI: 10.1016/j.carbpol.2018.06.112
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    Bio-inspired functionalization of microcrystalline cellulose aerogel with high adsorption performance toward dyes
    Wei, Xiao; Huang, Ting; Nie, Jun; Yang, Jing-hui; Qi, Xiao-dong; Zhou, Zuo-wan; Wang, Yong
    Carbohydrate Polymers (2018), 198 (), 546-555CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
    As one of the materials from natural resources, the functionalization and application of cellulose attract increasing concerns. In this work, we reported a facile method to prep. the bio-inspired functionalization of microcryst. cellulose (MCC) aerogel through polydopamine (PDA) coating, which was realized via the self-polymn. of dopamine in the MCC/LiBr soln. followed by the freeze-drying technol. The morphol. characterization showed that the pore morphologies of the compounded aerogel were influenced by the content of PDA. Adsorption measurements toward methylene blue (MB) showed that the compounded aerogel had high adsorption ability. Moreover, the compounded MCC/PDA aerogel exhibited excellent adsorption selectivity and it exhibited high efficiency to remove MB from different solns., such as the mixed soln. with anionic dyestuffs, the mixed soln. with cationic dyestuffs and the mixed soln. with common salt (NaCl). The high adsorption ability and excellent adsorption selectivity endows the compounded MCC/PDA aerogel with great potential applications in wastewater treatment.
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    Wan, C.; Zhang, L.; Yong, K.-T.; Li, J.; Wu, Y. Recent progress in flexible nanocellulosic structures for wearable piezoresistive strain sensors. J. Mater. Chem. C 2021, 9, 11001– 11029,  DOI: 10.1039/d1tc02360h
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    Recent progress in flexible nanocellulosic structures for wearable piezoresistive strain sensors
    Wan, Caichao; Zhang, Luyu; Yong, Ken-Tye; Li, Jian; Wu, Yiqiang
    Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2021), 9 (34), 11001-11029CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
    A review. With the coming of the "green" and "wearable" era, the superior flexibility and high biocompatibility accompanied by superb sensing abilities of nanocellulosic materials have significantly promoted the application of piezoresistive strain sensors in the area of intelligent wearable and skin-attachable devices (such as human motion detectors, human-machine interfaces, and electronic skins). In this review, a detailed overview on the design and prepn. strategies of nanocellulosic piezoresistive strain sensors is presented. The roles of nanocellulose in the core design parameters including sensitivity (gauge factor), dynamic durability, stretchability, hysteresis, and biocompatibility are summarized based on three primary points, namely the structure-response relationship, supramol. interaction, and synergistic mechanism. Furthermore, a comprehensive overview of the fundamental aspects related to the origin, physicochem. properties, and disassembly-reassembly approaches of nanocellulose is provided, and an anal. on the morphol. and mech. properties of 1D-to-3D nanocellulose assemblies is also illustrated. Finally, this review presents a brief summary, challenges, and perspectives of nanocellulosic strain sensors.
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    Wang, S.; Zhang, Q.; Wang, Z.; Pu, J. Facile fabrication of an effective nanocellulose-based aerogel and removal of methylene blue from aqueous system. J. Water Process Eng. 2020, 37, 101511,  DOI: 10.1016/j.jwpe.2020.101511
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    Nguyen, H. H. M.; Tan, K. V. M.; Van, T. T. T.; Nguyen, H. N.; Phan, A. N. Q.; Tran, A. T. T.; Le, P. K.; Le, K. A.; Nguyen, K. D.; Le, H. V. Preparation of Cu-modified bacterial cellulose aerogels derived from nata de coco towards the enhanced adsorption of hydrophobic organic solvents. J. Porous Mater. 2023, 30, 1195– 1205,  DOI: 10.1007/s10934-022-01413-z
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    Preparation of Cu-modified bacterial cellulose aerogels derived from nata de coco towards the enhanced adsorption of hydrophobic organic solvents
    Nguyen, Hanh H. M.; Tan, Khang V. M.; Van, Thanh T. T.; Nguyen, Hanh N.; Phan, Anh N. Q.; Tran, An T. T.; Le, Phung K.; Le, Kien A.; Nguyen, Khoa D.; Le, Ha V.
    Journal of Porous Materials (2023), 30 (4), 1195-1205CODEN: JPMAFX; ISSN:1380-2224. (Springer)
    This study presented a simple and eco-friendly method to load copper nanoparticles on the surface of bacterial cellulose from nata de coco produced via the fermn. of coconut water by Acetobacter xylinum. The Cu modification of BC surface was based on the redn. of copper (II) acetate by hydrazine under ambient conditions in a dispersion system of Nata de coco in water, which was followed by freeze-drying, affording lightwt. Cu-contg. cellulose aerogels. The structural features of the obtained aerogels were investigated by SEM with energy dispersive X-ray anal. (SEM/EDX), thermogravimetric anal. (TGA), powder X-ray diffraction (PXRD), and nitrogen physisorption, indicating the high cellulose crystallinity, three-dimensional matrix and homogenous dispersion of Cu species on the cellulose bundles. The Cu-modified aerogel exhibited a significantly improved adsorption capacity of cyclohexane (66.4 g/g) as compared to that of pure cellulose (45 g/g). The excellent performances of 65.1-109.6 g/g were also obsd. for other water-insol. liqs. including n-hexane, toluene, THF, Et acetate, chlorobenzene, 1,2-dichlorobenzene, dichloromethane, and chloroform depending their d.
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    Nath, P. C.; Ojha, A.; Debnath, S.; Neetu, K.; Bardhan, S.; Mitra, P.; Sharma, M.; Sridhar, K.; Nayak, P. K. Recent advances in valorization of pineapple (Ananas comosus) processing waste and by-products: A step towards circular bioeconomy. Trends Food Sci. Technol. 2023, 136, 100– 111,  DOI: 10.1016/j.tifs.2023.04.008
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    Recent advances in valorization of pineapple (Ananas comosus) processing waste and by-products: A step towards circular bioeconomy
    Nath, Pinku Chandra; Ojha, Amiya; Debnath, Shubhankar; Neetu, Kumari; Bardhan, Sayan; Mitra, Priya; Sharma, Minaxi; Sridhar, Kandi; Nayak, Prakash Kumar
    Trends in Food Science & Technology (2023), 136 (), 100-111CODEN: TFTEEH; ISSN:0924-2244. (Elsevier Ltd.)
    One of the most significant and challenging tasks on the planet is using fruit and vegetable wastes in the food processing industries. This waste disposal requires a substantial capital investment, the majority of which is for transportation. As a result, these wastes are dumped and burned in open areas. Thus, valorization strategies must be implemented in order to minimize the fruit and vegetables waste. This article reviewed the characteristics and nutritional compn. of pineapple wastes (PAWs), different waste parts of pineapple and their economic significance, utilization of high-value added products, and the benefits of employing PAWs in a variety of food applications. Pineapple has become a delicious fruit in recent times due to its unique aroma, an abundance of volatile chems., and nutritional content. The tropical fruit's pulp, skin, and leaves may provide a source of natural anti-microbial and antioxidant chems. From a socioeconomic point of view, PAW has the potential to become a new source of raw materials for the industries and could potentially replace the existing sources, which are both expensive and non-renewable. The bromelain enzyme extd. from pineapple and other key value-added products could be utilized in the food manufg. industry, thereby contributing to healthy food and a sustainable environment. Although studies have been conducted on a small scale, more investigation into the techno-economic viability of the biorefinery's processes is needed to ensure a smooth transition to a sustainable economy with minimal impact on the environment.
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    Meneses, I. P.; Novaes, S. D.; Dezotti, R. S.; Oliveira, P. V.; Petri, D. F. S. CTAB-modified carboxymethyl cellulose/bagasse cryogels for the efficient removal of bisphenol A, methylene blue and Cr(VI) ions: Batch and column adsorption studies. J. Hazard. Mater. 2022, 421, 126804,  DOI: 10.1016/j.jhazmat.2021.126804
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    CTAB-modified carboxymethyl cellulose/bagasse cryogels for the efficient removal of bisphenol A, methylene blue and Cr(VI) ions: Batch and column adsorption studies
    Meneses, Izabo Pereira; Novaes, Stephanie Dias; Dezotti, Rafael Sobral; Oliveira, Pedro Vitoriano; Petri, Denise Freitas Siqueira
    Journal of Hazardous Materials (2022), 421 (), 126804CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
    The simultaneous removal of org. and inorg. pollutants from water requires multifunctional adsorbents. Cryogels of CM-cellulose (CMC) and sugarcane bagasse (BG) were modified with cetyltrimethylammonium bromide (CTAB) micelles for the adsorption of methylene blue (MB), Cr(VI) ions and bisphenol A (BPA) sep., in binary or ternary aq. mixts. Batch adsorption studies of MB and Cr(VI) and BPA on the CMCBG-CTAB adsorbents indicated removal capacities of 100%, 70% and 95%, resp. MB adsorbed as multilayers on the CMCBG walls by electrostatic interaction, whereas Cr(VI) and BPA adsorbed on the cationic CTAB micelles surface and hydrophobic core of CTAB micelles, resp. The breakthrough curves obtained for pure adsorbates and their mixts. showed that the adsorption of Cr(VI) ions increased (i) ∼ 3.5 times in binary mixt. with BPA or in the ternary mixt., in comparison to pure Cr(VI) soln., and (ii) 1.4 times in binary mixt. with MB mols., due to synergistic effects. In the presence of Cr(VI) ions in binary or ternary mixts., the adsorption of MB was dramatically reduced due to screening effects. The adsorption of BPA was not significantly affected by the presence of MB or Cr(VI). The adsorbents were recycled five times without significant efficiency loss.
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    Liu, X.; Zhou, Y.; Nie, W.; Song, L.; Chen, P. Fabrication of hydrogel of hydroxypropyl cellulose (HPC) composited with graphene oxide and its application for methylene blue removal. J. Mater. Sci. 2015, 50, 6113– 6123,  DOI: 10.1007/s10853-015-9166-y
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    Fabrication of hydrogel of hydroxypropyl cellulose (HPC) composited with graphene oxide and its application for methylene blue removal
    Liu, Xiaoyan; Zhou, Yifeng; Nie, Wangyan; Song, Linyong; Chen, Pengpeng
    Journal of Materials Science (2015), 50 (18), 6113-6123CODEN: JMTSAS; ISSN:0022-2461. (Springer)
    Novel environmental friendly hydroxypropyl cellulose (HPC) hydrogels were fabricated upon compositing with graphene oxide (GO) in this work. In order to promote a more homogeneous dispersion of GO sheets in HPC, GO was firstly modified with HPC chains through esterification. The morphol. and chem. structure of the functionalized HPC-GO were characterized by transmission electron microscopy, XPS, Fourier transform IR spectrometer, X-ray diffraction, and thermo-gravimetric anal. Then scanning electronic microscope was employed to compare the morphologies of the HPC and HPC-GO/HPC hydrogels. The obtained HPC-GO/HPC hydrogels exhibited excellent adsorption performance toward methylene blue. Simulation of the practical use by prepg. simple adsorption columns made from in situ formation of HPC-based hydrogels had given a visible observation of the significant adsorption effect brought by the incorporation of HPC-GO sheets. Adsorption kinetics were then imitated by Lagergren pseudo-first-order and pseudo-second-order models. Adsorption isotherms were imitated by Langmuir isotherm and Freundlich isotherm.
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    Hua, J.; Meng, R.; Wang, T.; Gao, H.; Luo, Z.; Jin, Y.; Liu, L.; Yao, J. Highly Porous Cellulose Microbeads and their Adsorption for Methylene Blue. Fibers Polym. 2019, 20, 794– 803,  DOI: 10.1007/s12221-019-8334-0
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    Highly Porous Cellulose Microbeads and their Adsorption for Methylene Blue
    Hua, Jiarui; Meng, Ranju; Wang, Tiejun; Gao, Huiying; Luo, Zhenze; Jin, Yuanyuan; Liu, Lin; Yao, Juming
    Fibers and Polymers (2019), 20 (4), 794-803CODEN: FPIOA6; ISSN:1229-9197. (Korean Fiber Society)
    Highly porous cellulose microbeads with porosity of more than 90% were successfully prepd. via a facile dissoln. and subsequent regeneration of cellulose in H2SO4/Na2SO4 coagulation bath. Effects of coagulation temp., H2SO4, and Na2SO4 concn. on the microstructure, av. diam., porosity, sp. surface area, and mech. property of formed cellulose beads were investigated systematically. In view of the high porosity and specific area, the cellulose beads were used as adsorbents for dye removal. The results revealed that the porous cellulose beads exhibited high adsorption performance with max. adsorption capacity of 48.80 mg/g for cationic dye methylene blue. Besides, the porous cellulose beads also presented a potential in practical application and its adsorption capacity for methylene blue still retained 29.43 mg/g after six adsorption-desorption cycles.
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    Batzias, F.; Sidiras, D.; Schroeder, E.; Weber, C. Simulation of dye adsorption on hydrolyzed wheat straw in batch and fixed-bed systems. Chem. Eng. J. 2009, 148, 459– 472,  DOI: 10.1016/j.cej.2008.09.025
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    Simulation of dye adsorption on hydrolyzed wheat straw in batch and fixed-bed systems
    Batzias, Fragiskos; Sidiras, Dimitris; Schroeder, Elisabeth; Weber, Christina
    Chemical Engineering Journal (Amsterdam, Netherlands) (2009), 148 (2-3), 459-472CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
    The simulation of batch and column kinetics of Methylene Blue and Red Basic 22 adsorption on mild acid hydrolyzed wheat straw was investigated, using untreated wheat straw as control, in order to examine its properties for potential use as a low cost adsorbent for wastewater dye removal. The BET surface area, the adsorption capacities (estd. according to Freundlich and Langmuir models), indicated that mild acid hydrolysis enhances significantly the adsorption properties of the original material. This enhancement can be attributed to the removal of the hemicelluloses during sulfuric acid treatment, resulting in the opening' of the pores of lignocellulosic matrix's structure and the increasing of the BET surface area.
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    Mahmoud, M. E.; Abdelwahab, M. S. Fabricated and functionalized magnetite/phenylenediamine/cellulose acetate nanocomposite for adsorptive removal of methylene blue. Int. J. Biol. Macromol. 2019, 128, 196– 203,  DOI: 10.1016/j.ijbiomac.2019.01.102
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    Fabricated and functionalized magnetite/phenylenediamine/cellulose acetate nanocomposite for adsorptive removal of methylene blue
    Mahmoud, Mohamed E.; Abdelwahab, Mohamed S.
    International Journal of Biological Macromolecules (2019), 128 (), 196-203CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    The industrial revolution in textile and dying process is moving with huge steps, but the treatment of produced wastewater from this industry is a huge dilemma. This work demonstrates the prepn. and utilization of cellulose acetate (CA) blended with Fe3O4 already chem. modified with O-phenylenediamine (PDA) to prep. a novel magnetic Fe3O4/PDA/CA nanocomposite. This nanomaterial was aimed to use in the removal of methylene blue (MB) dye from water. The adsorption process was conducted using a batch technique and the removal process was evaluated under various exptl. conditions. From this study, it was found that the values were increased from 55.8% to 88.54%, 45.5% to 84.8% and 42.56% to 76.45% by the increase of from pH 1 to 7, resp. using 10, 50 and 100 mg·L-1. The pseudo-second-order was found to be the most fitted model to confirm that the adsorption reaction is related to a chemisorption process between the Fe3O4/PDA/CA nanocomposite and MB dye. The Langmuir and Freundlich models were also found to best-fitted models to reveal the formation of monolayer and multilayer of MB over Fe3O4/PDA/CA nanocomposite in a chem. process. The thermodn. parameters confirm that this type of reaction is spontaneous and exothermic reaction.
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    Shi, H.; Li, W.; Zhong, L.; Xu, C. Methylene Blue Adsorption from Aqueous Solution by Magnetic Cellulose/Graphene Oxide Composite: Equilibrium, Kinetics, and Thermodynamics. Ind. Eng. Chem. Res. 2014, 53, 1108– 1118,  DOI: 10.1021/ie4027154
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    Methylene Blue Adsorption from Aqueous Solution by Magnetic Cellulose/Graphene Oxide Composite: Equilibrium, Kinetics, and Thermodynamics
    Shi, Haochun; Li, Weisong; Zhong, Lei; Xu, Chunjian
    Industrial & Engineering Chemistry Research (2014), 53 (3), 1108-1118CODEN: IECRED; ISSN:0888-5885. (American Chemical Society)
    In the present study, magnetic cellulose/graphene oxide composite (MCGO) was prepd. as a novel adsorbent to dispose of dye wastewater. The morphol. and chem. structure of the MCGO composite were characterized by the Fourier transform IR spectrometer (FT-IR), X-ray diffraction (XRD), and scanning electronic microscope (SEM). The adsorption of methylene blue (MB) onto MCGO was studied in relation to initial concn. of MB, contact time, adsorbent dose, and pH value of soln. Adsorption kinetics and the equil. adsorption isotherm were fitted by a pseudo-second-order kinetic model and Langmuir isotherm, resp. The thermodn. parameters indicated that the adsorption was spontaneous, favorable, and exothermic in nature. Furthermore, MCGO was very stable and can easily be recycled. The adsorption efficiency of MCGO was still over 89% after recycling for five times.
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    Oyewo, O. A.; Adeniyi, A.; Sithole, B. B.; Onyango, M. S. Sawdust-Based Cellulose Nanocrystals Incorporated with ZnO Nanoparticles as Efficient Adsorption Media in the Removal of Methylene Blue Dye. ACS Omega 2020, 5, 18798– 18807,  DOI: 10.1021/acsomega.0c01924
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    Sawdust-based cellulose nanocrystals incorporated with ZnO nanoparticles as efficient adsorption media in the removal of methylene blue dye
    Oyewo, Opeyemi A.; Adeniyi, Amos; Sithole, B. Bruce; Onyango, Maurice S.
    ACS Omega (2020), 5 (30), 18798-18807CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    The continuous increase in the wastes generated from forestry, timber, and paper industries has engendered the need for their transformation into economically viable materials for the benefit of mankind. This study reports the prepn. and application of sawdust-derived cellulose nanocrystals (CNC) incorporated with zinc oxide as a novel adsorbent for the removal of methylene blue (MB) from water. The CNC/ZnO nanocomposite was characterized using Fourier transform IR, X-ray diffraction (XRD), and SEM. The amt. of MB adsorbed was detd. by a UV-vis spectrophotometer. The microscopic anal. revealed that the nanocomposite had a narrow particle size range and exhibited both spherical and rod-like morphologies. The XRD anal. of the nanocomposite showed characteristic high-intensity peaks in the range of 30-75° attributed to the presence of ZnO nanoparticles, which were responsible for the enhancement of the crystallinity of the nanocomposite. The results revealed a relationship between the MB removal efficiency and changes in soln. pH, nanocomposite dosage, initial concn., temp., and reaction time. The adsorption equil. isotherm, measured in the temp. range of 25-45 °C and using a concn. of 20-100 mg/L, showed that the MB sorption followed the Langmuir isotherm with a max. adsorption capacity of 64.93 mg/g. A pseudo-second-order kinetic model gave the best fit to the exptl. data. Based on adsorption performance, the CNC/ZnO nanocomposite offers prospects for further research and application in amelioration of dye-contg. effluent.
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    Safavi-Mirmahalleh, S.-A.; Salami-Kalajahi, M.; Roghani-Mamaqani, H. Effect of surface chemistry and content of nanocrystalline cellulose on removal of methylene blue from wastewater by poly(acrylic acid)/nanocrystalline cellulose nanocomposite hydrogels. Cellulose 2019, 26, 5603– 5619,  DOI: 10.1007/s10570-019-02490-1
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    Effect of surface chemistry and content of nanocrystalline cellulose on removal of methylene blue from wastewater by poly(acrylic acid)/nanocrystalline cellulose nanocomposite hydrogels
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    Cellulose (Dordrecht, Netherlands) (2019), 26 (9), 5603-5619CODEN: CELLE8; ISSN:0969-0239. (Springer)
    Nanocryst. cellulose (NCC) was modified with (3-aminopropyl)triethoxysilane (APTES) and hexadecyltrimethoxysilane (HDTMS) to obtain NCC-APTES and NCC-HDTMS resp. The modification was confirmed by Fourier transform IR (FT-IR) spectroscopy, X-ray diffraction (XRD) spectroscopy, thermogravimetric analyses (TGA), dynamic light scattering and zeta potential analyses. A series of poly(acrylic acid) (PAA)/NCC, PAA/NCC-APTES, and PAA/NCC-HDTMS hydrogel nanocomposites with various amts. of nanoparticles were synthesized by in situ radical polymn. method. Nanocomposites were characterized using XRD, TGA and field emission SEM. Also, swelling behavior of hydrogel nanocomposites showed that NCC and NCC-APTES helped swelling of hydrogels whereas CNN-HDTMS decreased swelling ratio. The hydrogel nanocomposites were also used as adsorbents for removal of methylene Blue from aq. soln. at different pH values. Results showed that the adsorption capacity for dye increased with increasing pH and contact time. Introducing NCC into hydrogel nanocomposite network affected adsorption capacity. Finally, adsorption kinetics was studied by three kinetic models including pseudo-first-order, pseudo-second-order and intra-particle diffusion models.
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    Cheng, J.; Zhan, C.; Wu, J.; Cui, Z.; Si, J.; Wang, Q.; Peng, X.; Turng, L.-S. Highly Efficient Removal of Methylene Blue Dye from an Aqueous Solution Using Cellulose Acetate Nanofibrous Membranes Modified by Polydopamine. ACS Omega 2020, 5, 5389– 5400,  DOI: 10.1021/acsomega.9b04425
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    Highly Efficient Removal of Methylene Blue Dye from an Aqueous Solution Using Cellulose Acetate Nanofibrous Membranes Modified by Polydopamine
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    ACS Omega (2020), 5 (10), 5389-5400CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    A new type of deacetylated cellulose acetate (DA)@polydopamine (PDA) composite nanofiber membrane was fabricated by electrospinning and surface modification. The membrane was applied as a highly efficient adsorbent for removing methylene blue (MB) from an aq. soln. The morphol., surface chem., surface wettability, and effects of operating conditions on MB adsorption ability, as well as the equil., kinetics, thermodn., and mechanism of adsorption, were systematically studied. The results demonstrated that a uniform PDA coating layer was successfully developed on the surface of DA nanofibers. The adsorption capacity of the DA@PDA nanofiber membrane reached up to 88.2 mg/g at a temp. of 25°C and a pH of 6.5 after adsorption for 30 h, which is about 8.6 times higher than that of DA nanofibers. The exptl. results showed that the adsorption behavior of DA@PDA composite nanofibers followed the Weber's intraparticle diffusion model, pseudo-second-order model, and Langmuir isothermal model. A thermodn. anal. indicated that endothermic, spontaneous, and physisorption processes occurred. Based on the exptl. results, the adsorption mechanism of DA@PDA composite nanofibers was also demonstrated.
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    Fang, Y.; Liu, Q.; Zhu, S. Selective biosorption mechanism of methylene blue by a novel and reusable sugar beet pulp cellulose/sodium alginate/iron hydroxide composite hydrogel. Int. J. Biol. Macromol. 2021, 188, 993– 1002,  DOI: 10.1016/j.ijbiomac.2021.07.192
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    Selective biosorption mechanism of methylene blue by a novel and reusable sugar beet pulp cellulose/sodium alginate/iron hydroxide composite hydrogel
    Fang, Yi; Liu, Qiang; Zhu, Siming
    International Journal of Biological Macromolecules (2021), 188 (), 993-1002CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    A cellulose-based sodium alginate/iron hydroxide (C/SA/Fe) composite hydrogel was fabricated by using epichlorohydrin as crosslinking agent as an effective adsorbent for dye. The physicochem. structure of the C/SA/Fe hydrogel was characterized by SEM, FTIR, XRD and TG. The adsorption performance for the removal of methylene blue (MB) was investigated. In addn., the selective adsorption of cationic dye was also studied. The FTIR anal. revealed that the Fe(OH)3 colloidal particles were successfully combined in the cellulose/sodium alginate hydrogel. The modified hydrogel had better adsorption performance, and the max. adsorption capacity of C/SA/Fe0.5 for MB was 105.93 mg/g according to the fitting results of adsorption isotherm. The kinetic study showed that the adsorption of MB onto C/SA/Fe was more consistent with the pseudo-second-order model, and was dominated by chemisorption mechanism such as ion exchange or electron sharing. The adsorption data fits well with the Langmuir model. Thermodn. anal. showed that the MB adsorption by C/SA/Fe was exothermic, spontaneous, favorable and feasible. After five adsorption-desorption cycles, the adsorption capacity was almost unchanged. So, the C/SA/Fe hydrogel is a potential material in the field of the recovery of agricultural byproducts or other bio-based cellulose, or environmental protection, etc.
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    Cao, X.; Liu, M.; Bi, W.; Lin, J.; Chen, D. D. Y. Direct carboxylation of cellulose in deep eutectic solvent and its adsorption behavior of methylene blue. Carbohydr. Polym. Technol. Appl. 2022, 4, 100222,  DOI: 10.1016/j.carpta.2022.100222
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    Direct carboxylation of cellulose in deep eutectic solvent and its adsorption behavior of methylene blue
    Cao, Xiwang; Liu, Min; Bi, Wentao; Lin, Jun; Chen, David Da Yong
    Carbohydrate Polymer Technologies and Applications (2022), 4 (), 100222CODEN: CPTACM; ISSN:2666-8939. (Elsevier Ltd.)
    The surface of cellulose particles was carboxylated (2.44 mmol/g) in a deep eutectic solvent contg. carboxylic acid. Based on the carboxyl content, the effects of key factors on cellulose carboxylation was systematically investigated. In addn., the reaction mechanism was studied by using liq. chromatog.-mass spectrometry, and the influence of deep eutectic solvent contg. carboxylic acid on the structure and physicochem. properties of cellulose during carboxylation was examd. using different characterization techniques. The results showed that the type of carboxylic acid, cellulose particle size, and pretreatment methods significantly affect the carboxylation efficiency, degrdn., and carbonization of cellulose. The internal crystal structure of cellulose did not change after the carboxylation reaction, while the surface crystal structure was destroyed by carboxylation, which greatly improved the dispersion and hydrophilicity properties of the product. The kinetics and thermodn. of carboxyl cellulose adsorption were studied as well. Potential application of carboxyl cellulose in the adsorption of pollutants was demonstrated. This study provides a new method for the direct modification of cellulose in deep eutectic solvents, as well as a new sustainable strategy for modifying other materials.
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    Beh, J. H.; Lim, T. H.; Lew, J. H.; Lai, J. C. Cellulose nanofibril-based aerogel derived from sago pith waste and its application on methylene blue removal. Int. J. Biol. Macromol. 2020, 160, 836– 845,  DOI: 10.1016/j.ijbiomac.2020.05.227
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    Cellulose nanofibril-based aerogel derived from sago pith waste and its application on methylene blue removal
    Beh, Jeng Hua; Lim, Teck Hock; Lew, Jin Hau; Lai, Jau Choy
    International Journal of Biological Macromolecules (2020), 160 (), 836-845CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
    Sago pith cellulose nanofibril (SPCNF) aerogel derived from sago pith waste (SPW) was successfully produced through three consecutive steps, namely dewaxing and delignification, ultra-sonication and homogenization and freeze drying. The aerogel was characterized using field emission SEM (FE-SEM), Fourier-transform infra-red spectroscopy (FTIR), X-ray diffraction (XRD) and thermogravimetric anal. (TGA). Results of the analyses collectively showed that lignin & hemicellulose were absent in the SPCNF aerogel product which has a high crystallinity index of 88%. The diams. of individual nanofibril constituents of the SPCNF were between 15 and 30 nm and aspect ratios >1000 were obsd. The SPCNF aerogel, with a d. measured at 2.1 mg/cm3, was efficient in methylene blue (MB) removal with a max. MB adsorption of 222.2 mg/g at 20°C. The adsorption of MB onto the SPCNF aerogel was rapid and found to follow a pseudo-second-order kinetic model with the adsorption isotherm being in congruence with the Langmuir model. The SPCNF aerogel exhibited outstanding MB removal efficacies with 5 mg and 20 mg of SPCNF capable of removing over 90% and almost 99% MB, resp. The optimized pH value and temp. for MB adsorption were detd. as pH 7 and 20°C.
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    Chong, K. Y.; Chia, C. H.; Zakaria, S.; Sajab, M. S.; Chook, S. W.; Khiew, P. S. CaCO3-decorated cellulose aerogel for removal of Congo Red from aqueous solution. Cellulose 2015, 22, 2683– 2691,  DOI: 10.1007/s10570-015-0675-2
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    CaCO3-decorated cellulose aerogel for removal of Congo Red from aqueous solution
    Chong, Kai Yin; Chia, Chin Hua; Zakaria, Sarani; Sajab, Mohd. Shaiful; Chook, Soon Wei; Khiew, Poi Sim
    Cellulose (Dordrecht, Netherlands) (2015), 22 (4), 2683-2691CODEN: CELLE8; ISSN:0969-0239. (Springer)
    The present study describes the prepn. of CaCO3-loaded cellulose aerogel and evaluation of its adsorptive removal of Congo Red (CR) from aq. soln. The CaCO3-cellulose aerogel was produced via in situ pptn. of CaCO3 into as-prepd. cellulose aerogel, which was prepd. by freeze-drying a crosslinked cellulose soln. that was dissolved using a NaOH/urea soln. The particles that formed in the aerogel were confirmed to be calcite CaCO3. Adsorption studies illustrated that the CR uptake by the aerogel was dependent on the dye concn. and temp. Incorporation of CaCO3 into the cellulose aerogel significantly enhanced the adsorption capacity of the aerogel toward CR. The max. adsorption capacity of the CaCO3-cellulose aerogel was approx. 75.81 mg/g.
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    Abramian, L.; El-Rassy, H. Adsorption kinetics and thermodynamics of azo-dye Orange II onto highly porous titania aerogel. Chem. Eng. J. 2009, 150, 403– 410,  DOI: 10.1016/j.cej.2009.01.019
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    Adsorption kinetics and thermodynamics of azo-dye Orange II onto highly porous titania aerogel
    Abramian, Lara; El-Rassy, Houssam
    Chemical Engineering Journal (Amsterdam, Netherlands) (2009), 150 (2-3), 403-410CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
    We report herein a kinetic and thermodn. study of the adsorption of azo-dye Orange II from aq. solns. onto titania aerogels. Aerogels structure was confirmed by FTIR and N2 adsorption revealed their sp. surface area (500 m2/g), pore vol. (2.86 cm3/g) and pore size (mean 13.9 nm). Adsorption tests were conducted in batch reactors under various conditions where the effect of pH, temp., contact time, dye concn., and adsorbent dose were studied. Expts. performed at pH 2 show the optimal adsorption due to the best surface charge interactions. The temp. shows a weak influence with a decrease in the adsorption uptake as the temp. increases. Adsorption kinetics is shown to be very fast and follows a pseudo second-order indicating the coexistence of chemisorption and physisorption with the intra-particle diffusion being the rate controlling step. The exptl. data fit perfectly with Sips isotherms and reveal the ability of titania aerogel to adsorb 420 mg of Orange II per g of adsorbent at the optimal conditions. The thermodn. study reveals the activation energy (42.1 kJ/mol-1) and the changes in Gibbs free energy (1.2 kJ/mol-1), enthalpy (-16.4 kJ/mol-1), and entropy (-58 J/mol-1/K-1). The entire regeneration of the titania aerogel adsorption sites at pH 11 and 30° shows a total recovery of the dye and the efficient reusability and the economic interest of these adsorbing materials for environmental purposes.
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  5. Uun Yanuhar, Heru Suryanto, Husni Wahyu Wijaya, Joseph Selvi Binoj, Aminnudin Aminnudin, Nico Rahman Caesar, Azlin Fazlina Osman, Fajar Nusantara, Inpita Casuarina Eqisetia Utari. Membrane Derived from Pineapple Biowaste for Water Filtration in Aquaculture Environment: Effect of Zinc Oxide Nanoparticle. Case Studies in Chemical and Environmental Engineering 2025, 17 , 101114. https://doi.org/10.1016/j.cscee.2025.101114
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  8. Alireza Ashori, Elahe Chiani, Soheila Shokrollahzadeh, Meysam Madadi, Fubao Sun, Xueming Zhang. Cellulose-Based Aerogels for Sustainable Dye Removal: Advances and Prospects. Journal of Polymers and the Environment 2024, 32 (12) , 6149-6181. https://doi.org/10.1007/s10924-024-03394-3
  9. Phuong X.T. Nguyen, Anh P.N. Pham, Hong T.T. Nguyen, Tai C. Do, Phung K. Le. Flexible aerogel composites for the elimination of crystal violet and methyl orange. Journal of Porous Materials 2024, 31 (6) , 2003-2016. https://doi.org/10.1007/s10934-024-01654-0
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  12. Yue Wang, Tingting Zhang, Meizi Huang, Ming Zhang, Yu-Cai He. Preparation of dandelion flower extract-based polyvinyl alcohol-chitosan-dandelion-CuNPs composite gel for efficient bacteriostatic and dye adsorption. International Journal of Biological Macromolecules 2024, 281 , 136512. https://doi.org/10.1016/j.ijbiomac.2024.136512
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  15. O Oktaviani, A R Syahputra, A L Yunus, N Nuryanthi, A Nilatany, T Puspitasari, R Maryana. Amidoximated Bacterial Cellulose Film for Pb 2+ Adsorption in Aqueous Environment. Journal of Physics: Conference Series 2024, 2828 (1) , 012046. https://doi.org/10.1088/1742-6596/2828/1/012046
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  19. Ngoan Thi Thao Nguyen, Luan Minh Nguyen, Thuy Thi Thanh Nguyen, Duyen Thi Cam Nguyen, Thuan Van Tran. Synthesis strategies, regeneration, cost analysis, challenges and future prospects of bacterial cellulose-based aerogels for water treatment: A review. Chemosphere 2024, 362 , 142654. https://doi.org/10.1016/j.chemosphere.2024.142654
  20. Faezeh Karami, Hassan Sereshti. Ultrasonic-induced grafted lanthanum sulfide decorated multi-walled carbon nanotube onto bacterial cellulose applied for adsorption of pesticides in environmental waters. Journal of Chromatography A 2024, 1727 , 464976. https://doi.org/10.1016/j.chroma.2024.464976
  21. Tian Mai, Pei-Lin Wang, Ming-Guo Ma. Promising cellulose-based aerogel composites: Preparation methods and advanced applications. Composites Part B: Engineering 2024, 281 , 111559. https://doi.org/10.1016/j.compositesb.2024.111559
  22. Haize Su, Tianren Deng, Weipeng Qiu, Tenggen Hu, Xiaoling Zheng, Kaibin Peng, Yingyuan Zhang, Yali Zhao, Zhenlin Xu, Hongtao Lei, Hong Wang, Peng Wen. One stone, two birds: An eco-friendly aerogel based on waste pomelo peel cellulose for the efficient adsorption of dyes and heavy metal ions. International Journal of Biological Macromolecules 2024, 273 , 132875. https://doi.org/10.1016/j.ijbiomac.2024.132875
  23. Phuong X.T. Nguyen, Anh P.N. Pham, Hong T.T. Nguyen, Tai C. Do, Phung K. Le. Flexible aerogel composites for the elimination of crystal violet and methyl orange. 2024https://doi.org/10.21203/rs.3.rs-4463585/v1
  24. Siriporn Taokaew. Bacterial Nanocellulose Produced by Cost-Effective and Sustainable Methods and Its Applications: A Review. Fermentation 2024, 10 (6) , 316. https://doi.org/10.3390/fermentation10060316
  25. Ha V. Le, Nhi T. Vo, Hoan T. Phan, Thu M. Dao, Bao G. Nguyen, Tung T. Nguyen, Phuoc H. Ho, Khoa D. Nguyen. A sulfonate ligand-defected Zr-based metal–organic framework for the enhanced selective removal of anionic dyes. RSC Advances 2024, 14 (23) , 16389-16399. https://doi.org/10.1039/D4RA02803A
  26. Sahil Chaudhary, Barinderjit Singh. Pineapple by-products utilization: Progress towards the circular economy. Food and Humanity 2024, 2 , 100243. https://doi.org/10.1016/j.foohum.2024.100243
  27. Prakash Kumar Sarangi, Rajesh Kumar Srivastava, Uttam Kumar Sahoo, Akhilesh Kumar Singh, Jigisha Parikh, Shama Bansod, Ganesh Parsai, Mohammad Luqman, Krushna Prasad Shadangi, Deepti Diwan, Deborah Lanterbecq, Minaxi Sharma. Biotechnological innovations in nanocellulose production from waste biomass with a focus on pineapple waste. Chemosphere 2024, 349 , 140833. https://doi.org/10.1016/j.chemosphere.2023.140833
  28. Tian Mai, Peilin Wang, Mingguo Ma. Promising cellulose-based aerogel composites: Preparation methods and advanced applications. 2024, 289-327. https://doi.org/10.1016/B978-0-443-13675-7.00009-9
  29. Hassan Sereshti, Faezeh Karami. Ultrasonic-Induced Grafted Lanthanum Sulfide Decorated Multi-Walled Carbon Nanotube Onto Bacterial Cellulose for Green Adsorption of Multiclass Pesticides in Environmental Waters. 2024https://doi.org/10.2139/ssrn.4756164
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Cite this: ACS Omega 2023, 8, 37, 33412–33425
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Published September 1, 2023

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  • Abstract

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    Figure 1

    Figure 1. Photographs of (a) 100-g batch of the nata de pina preparation via the fermentation of the extract of pineapple peel waste and (b) nata de pina after washing with NaOH and water, sequentially.

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    Figure 2

    Figure 2. Characterizations of the aerogel material derived from pineapple peel waste: PXRD pattern (a); SEM image (b); N2 physisorption isotherm (c); and pore size distribution (d).

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    Figure 3

    Figure 3. TGA profiles of the fresh BC aerogel (a) and the BC sample after the adsorption experiment with a 50-ppm solution of MB for 30 min (b).

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    Figure 4

    Figure 4. Effect of temperature on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at pH = 6.5 for 30 min.

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    Figure 5

    Figure 5. Effect of adsorption time on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at 30 °C, and pH = 6.5.

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    Figure 6

    Figure 6. (a) First-order and (b) second-order adsorption kinetics of the methylene blue adsorption using the bacterial cellulose aerogel material.

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    Figure 7

    Figure 7. Proposal of adsorptive sites and their interactions with methylene blue molecules at different pH values.

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    Figure 8

    Figure 8. Effect of the pH value on methylene blue adsorption capacity. Adsorption conditions: 20 mg of aerogel, 10 mL of 50 ppm MB solution at 30 °C for 30 min.

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    Figure 9

    Figure 9. Effect of initial methylene blue concentration on adsorption capacity. Adsorption condition: 20 mg of aerogel, 10 mL of MB solution at 30 °C for 30 min and pH = 6.5.

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    Figure 10

    Figure 10. MB adsorption isotherms of the BC aerogel derived from pineapple peel waste fitted by Langmuir model (a) and Freundlich model (b).

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    Figure 11

    Figure 11. Photographs of aerogel samples prepared from the suspensions with varied BC concentrations (a) and their effect on the adsorption capacity and the specific surface area of the obtained aerogels (b).

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    Figure 12

    Figure 12. Methylene blue adsorption capacity on the aerogel samples prepared from the suspensions with different sizes of nata de pina hydrogel particles. Adsorption condition: 20 mg of aerogel, 10 mL of MB solution with a concentration of 200 ppm, at 30 °C for 30 min and pH = 6.5.

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    Figure 13

    Figure 13. Adsorption capacity of the aerogel for various organic dyes. Adsorption condition: 20 mg of aerogel, 10 mL of dye solution with a concentration of 200 ppm, at 30 °C and pH = 6.5 for 30 min.

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    Figure 14

    Figure 14. Effect of aqueous solution volume on methylene blue adsorption capacity of the aerogel and recycling test employing cellulose-based aerogel in the removal of methylene blue (*). Adsorption condition: solid/liquid ratio = 2 mg/1 mL with a concentration of 200 ppm MB, at 30 °C and pH = 6.5 for 30 min.

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      High adsorption performance of β-cyclodextrin-functionalized multi-walled carbon nanotubes for the removal of organic dyes from water and industrial wastewater
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      Removal of inorg. and org. pollutants from synthetic and industrial wastewater samples is one of the biggest challenges facing researchers. In this work, glycine-β-cyclodextrin-functionalized carbon nanotubes (MWCNTs/Gly/β-CD) as a novel nano-adsorbent were synthesized and developed for the removal of org. pollutants. The structure and morphol. of MWCNTs/Gly/β-CD was characterized by FT-IR, FESEM, TEM, XRD and EDX, and the results showed that the MWCNT was modified with Gly and β-CD. The effects of surface improvement on the adsorption of org. pollutants were studied in a batch system by considering various parameters such as contact time, adsorbent dosage, pH, and temp. The results indicated that the max. capacities of MB, AB113, MO and DR1 onto MWCNTs/Gly/β-CD were 90.90mg g-1, 172.41mg g-1, 96.15mg g-1, and 500mg g-1, resp. The dye adsorption kinetics, thermodn. and isotherms were also investigated. The results indicated that pseudo-second-order kinetics model (R2 > 0.999) and Langmuir isotherm model (R2 > 0.995) well describe the adsorption of the tested dyes on the MWCNTs/Gly/β-CD. In comparison with the raw MWCNTs and MWCNTs/Gly samples, the dye removal efficiency was increased for the synthesized MWCNTs/Gly/β-CD nano-adsorbent. Our results confirmed that β-CD-functionalized MWCNTs can be used as an effective adsorbent due to the high adsorption capacity of dyes as well as the short equil. time needed. Therefore, MWCNTs/Gly/β-CD was successfully applied to remove org. pollutants from synthetic and industrial wastewater samples with excellent results.
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      Xiao, W.; Jiang, X.; Liu, X.; Zhou, W.; Garba, Z. N.; Lawan, I.; Wang, L.; Yuan, Z. Adsorption of organic dyes from wastewater by metal-doped porous carbon materials. J. Cleaner Prod. 2021, 284, 124773,  DOI: 10.1016/j.jclepro.2020.124773
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      A review. In this review paper, the recent development on the adsorption of org. dyes by metal-doped porous carbon materials were reviewed. The primary objective of this paper is to sort out the dispersion information of metal-doped porous carbon materials widely used in org. dye adsorption. Various metal-doped porous carbon materials adsorbing org. dyes are summarized and discussed here for the first time. Key factors affecting the adsorption process such as the amt. of doped metal, soln. pH, and temp. are also reported and discussed. The adsorption mechanisms such as electrostatic interaction, π-π interaction, hydrogen bonding and synergistic interaction between metal particles and carbon materials are proposed for org. dyes adsorption on metal-doped porous carbon with the help of related works from the literature. Finally, few suggestions for future studies on metal-doped porous carbon materials are proposed.
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      Nguyen, K. D.; Ho, P. H.; Vu, P. D.; Pham, T. L. D.; Trens, P.; Di Renzo, F.; Phan, N. T. S.; Le, H. V. Efficient Removal of Chromium(VI) Anionic Species and Dye Anions from Water Using MOF-808 Materials Synthesized with the Assistance of Formic Acid. Nanomaterials 2021, 11, 1398,  DOI: 10.3390/nano11061398
      10
      Efficient removal of chromium(VI) anionic species and dye anions from water using mof-808 materials synthesized with the assistance of formic acid
      Nguyen, Khoa D.; Ho, Phuoc H.; Vu, Phuong D.; Pham, Thuyet L. D.; Trens, Philippe; Renzo, Francesco Di; Phan, Nam T. S.; Le, Ha V.
      Nanomaterials (2021), 11 (6), 1398CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
      This study presents a simple approach to prep. MOF-808, an ultra-stable Zr-MOF constructed from 6-connected zirconium clusters and 1,3,5-benzene tricarboxylic acid, with tailored particle sizes. Varying the amt. of formic acid as a modulator in the range of 200-500 equiv results in MOF-808 materials with a crystal size from 40 nm to approx. 1000 nm. Apart from the high sp. surface area, a combination of a fraction of mesopore and plenty of acidic centers on the Zr-clusters induces a better interaction with the ionic pollutants such as K2Cr2O7 and anionic dyes. MOF-808 shows uptakes of up to 141.2, 642.0, and 731.0 mg/g for K2Cr2O7, sunset yellow, and quinoline yellow, resp., in aq. solns. at ambient conditions. The uptakes for the ionic dyes are significantly higher than those of other MOFs reported from the literature. Moreover, the adsorption capacity of MOF-808 remains stable after four cycles. Our results demonstrate that MOF-808 is a promising ideal platform for removing oxometallates and anionic dyes from water.
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      A review. The contamination of groundwater by heavy metal, originating either from natural soil sources or from anthropogenic sources is a matter of utmost concern to the public health. Remediation of contaminated groundwater is of highest priority since billions of people all over the world use it for drinking purpose. In this paper, thirty five approaches for groundwater treatment have been reviewed and classified under three large categories viz chem., biochem./biol./biosorption and physico-chem. treatment processes. Comparison tables have been provided at the end of each process for a better understanding of each category. Selection of a suitable technol. for contamination remediation at a particular site is one of the most challenging job due to extremely complex soil chem. and aquifer characteristics and no thumb-rule can be suggested regarding this issue. In the past decade, iron based technologies, microbial remediation, biol. sulfate redn. and various adsorbents played versatile and efficient remediation roles. Keeping the sustainability issues and environmental ethics in mind, the technologies encompassing natural chem., bioremediation and biosorption are recommended to be adopted in appropriate cases. In many places, two or more techniques can work synergistically for better results. Processes such as chelate extn. and chem. soil washings are advisable only for recovery of valuable metals in highly contaminated industrial sites depending on economical feasibility. Various technologies for remediating heavy metal contaminated groundwater has been reviewed.
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      Maleki, Hajar
      Chemical Engineering Journal (Amsterdam, Netherlands) (2016), 300 (), 98-118CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
      A review concerning recent advances in aerogel synthesis, processing, and air and water purifn. adsorption applications is given. Topics discussed include: introduction; synthesis (sol-gel process, aging, drying [supercrit., ambient pressure, freeze], carbonization, carbo-thermal redn. to prep. carbide aerogels); aerogel air purifn. applications (CO2 capture, volatile org. compd. removal); aerogel water purifn. applications (oil and toxic org. pollutant clean-up, heavy metal ion removal); and conclusions and outlook. Although, aerogel environmental remediation performance is promising, some drawbacks (an intricate drying process, mech. delicate structure, processing cost) were examd. and were abated in some manner in several studies.
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    16. 16
      Wang, Y.; Su, Y.; Wang, W.; Fang, Y.; Riffat, S. B.; Jiang, F. The advances of polysaccharide-based aerogels: Preparation and potential application. Carbohydr. Polym. 2019, 226, 115242,  DOI: 10.1016/j.carbpol.2019.115242
      16
      The advances of polysaccharide-based aerogels: Preparation and potential application
      Wang, Yixin; Su, Yuehong; Wang, Weiling; Fang, Ying; Riffat, Saffa B.; Jiang, Fatang
      Carbohydrate Polymers (2019), 226 (), 115242CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
      A review. Polysaccharide-based aerogels have high application value as one kind of unique functional materials. Not only has it high porosity and low-d., but also the non-toxicity and biodegradability. In recent decades, a variety of natural raw materials and their combinations along with various prepn. technologies have been investigated to develop polysaccharide-based aerogels with different functions for diverse applications. This review aims to clarify a general approach in the development of polysaccharide-based aerogels regarding pore structure design, polysaccharide selection and drying methods. The relevant researches and reports of polysaccharide-based aerogels have been also classified according to the applications in environmental engineering, buildings, medical practice, packaging and electrochem. Furthermore, some statistical graphs have been produced to summarize those publications during the past ten years, with an aim to indicate the distribution and research trend. Finally, the approaches to improve the quality of the aerogels are discussed and some perspectives are put forward to provide a ref. for the future development of polysaccharide-based aerogels.
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    17. 17
      Chen, X.; Cui, J.; Xu, X.; Sun, B.; Zhang, L.; Dong, W.; Chen, C.; Sun, D. Bacterial cellulose/attapulgite magnetic composites as an efficient adsorbent for heavy metal ions and dye treatment. Carbohydr. Polym. 2020, 229, 115512,  DOI: 10.1016/j.carbpol.2019.115512
      17
      Bacterial cellulose/attapulgite magnetic composites as an efficient adsorbent for heavy metal ions and dye treatment
      Chen, Xiao; Cui, Jian; Xu, Xuran; Sun, Bianjing; Zhang, Lei; Dong, Wei; Chen, Chuntao; Sun, Dongping
      Carbohydrate Polymers (2020), 229 (), 115512CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
      In recent decades, increased industrial activities led to the release of various pollutants, such as toxic heavy metals, inorg. anions, and orgs. It is imperative but challenging to develop an eco-friendly treatment technol. with easy operation, low cost, and high efficiency. Here, we describe a design of magnetic purifier, which has biomass-based structure by blending attapulgite/chitosan (ATP/CS) composite with bacterial cellulose nanofibrils (BCNs). Compared to similar materials reported previously, the product exhibited efficient adsorption capacities towards various metal ions including Pb2+, Cu2+, and Cr6+, and anionic org. dyes including Congo red. The adsorption process could be well fitted by Langmuir isotherm and pseudo-second order equation. Addnl., the adsorption capacity only decreased <8% after 5 adsorption-desorption cycles. We expect the design will inspire more efforts to build a multifunctional H2O purifier with simple operation, and hopefully effectively remove pollutants from wastewater in future practical applications.
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    18. 18
      Budtova, T. Cellulose II aerogels: a review. Cellulose 2019, 26, 81– 121,  DOI: 10.1007/s10570-018-2189-1
      18
      Cellulose II aerogels: a review
      Budtova, Tatiana
      Cellulose (Dordrecht, Netherlands) (2019), 26 (1), 81-121CODEN: CELLE8; ISSN:0969-0239. (Springer)
      A review. Cellulose II aerogels are light-wt., open pores materials with high sp. surface area. They are made in the same way as bio-aerogels based on other polysaccharides, via dissoln.-(gelation)-solvent exchange-drying with supercrit. CO2. Gelation step is often omitted as cellulose allows keeping 3D shape during solvent exchange (which leads to cellulose coagulation) and drying. Drying in supercrit. conditions preserves the porosity of "wet" (coagulated) cellulose. There are numerous ways to vary cellulose II aerogel morphol. and properties by changing processing conditions and cellulose type. Together with chem. and phys. modifications of cellulose and possibility of making hybrid and composite materials (org.-inorg. and org.-org.), it opens up a huge variety of aerogel properties and applications. On one hand, they are similar to those of classical aerogels, i.e. can be used for absorption and adsorption, as catalysts and catalysts support and in electro-chem. when pyrolyzed. On the other hand, because the prepn. of cellulose aerogels may not involve any toxic compds., they can be used in life science applications such as pharma, bio-medical, food and cosmetics. The review makes an overview of results reported in literature on the structure and properties of cellulose II aerogels and their applications. The reader may be surprised finding more questions than answers and clear trends. The review shows that several fundamental questions still remain to be answered and applications to be explored.
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    19. 19
      Galiwango, E.; Abdel Rahman, N. S.; Al-Marzouqi, A. H.; Abu-Omar, M. M.; Khaleel, A. A. Isolation and characterization of cellulose and α-cellulose from date palm biomass waste. Heliyon 2019, 5, e02937  DOI: 10.1016/j.heliyon.2019.e02937
      There is no corresponding record for this reference.
    20. 20
      Wang, N.; Xu, B.; Wang, X.; Lang, J.; Zhang, H. Chemical and Structural Elucidation of Lignin and Cellulose Isolated Using DES from Bagasse Based on Alkaline and Hydrothermal Pretreatment. Polymers 2022, 14, 2756,  DOI: 10.3390/polym14142756
      20
      Chemical and Structural Elucidation of Lignin and Cellulose Isolated Using DES from Bagasse Based on Alkaline and Hydrothermal Pretreatment
      Wang, Na; Xu, Baoming; Wang, Xinhui; Lang, Jinyan; Zhang, Heng
      Polymers (Basel, Switzerland) (2022), 14 (14), 2756CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
      The sepn. of cellulose, hemicellulose, and lignin components using deep eutectic solvent, which is a green solvent, to obtain corresponding chems. can realize the effective sepn. and high-value utilization of these components at low cost. In this study, we used waste biomass sugarcane bagasse as the raw material, choline chloride as the hydrogen bond acceptor, and lactic acid as the hydrogen bond donor to synthesize a deep eutectic solvent of choline chloride/lactic acid (L-DES) and treated sugarcane bagasse pretreated by alkali or hydrothermal methods to sep. cellulose, hemicellulose, and lignin. In addn., we comparatively studied the effect of different pretreatment methods on lignin removal by DES and found that the lignin removal rate by L-DES after alk. pretreatment was significantly higher than that after hydrothermal pretreatment, and the mechanism of action causing this difference is discussed.
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    21. 21
      Rehman, N.; Alam, S.; Amin, N. U.; Mian, I.; Ullah, H. Ecofriendly Isolation of Cellulose from Eucalyptus lenceolata: A Novel Approach. Int. J. Polym. Sci. 2018, 2018, 8381501– 7,  DOI: 10.1155/2018/8381501
      There is no corresponding record for this reference.
    22. 22
      Urbina, L.; Corcuera, M. Á.; Gabilondo, N.; Eceiza, A.; Retegi, A. A review of bacterial cellulose: sustainable production from agricultural waste and applications in various fields. Cellulose 2021, 28, 8229– 8253,  DOI: 10.1007/s10570-021-04020-4
      22
      A review of bacterial cellulose: sustainable production from agricultural waste and applications in various fields
      Urbina, Leire; Corcuera, Maria Angeles; Gabilondo, Nagore; Eceiza, Arantxa; Retegi, Alona
      Cellulose (Dordrecht, Netherlands) (2021), 28 (13), 8229-8253CODEN: CELLE8; ISSN:0969-0239. (Springer)
      A review. Bacterial cellulose (BC) is a polymer with interesting conformation and properties. BC can be obtained in different shapes and is easily modified by chem. and phys. means, so its applications in the prodn. of new materials and nanocomposites for different purposes have been in the focus of many research projects. However, one of the major challenges to address in bacterium-derived polymer technol. is to find suitable carbon sources as substrates that are cheap and do not compete with food prodn. for achieving large scale industrial applications. Agricultural wastes are defined as the residues from the growing and processing of raw agricultural products such as crops, fruits, vegetables and dairy products. Their compn. can vary depending on the type of agricultural activity and harvesting conditions, but these residues are suitable for the prodn. of BC. The aim of this review is to give insight into the prodn. of BC using agro-wastes and an overview of the most interesting and novel applications of this biopolymer in different areas i.e. environmental applications, optoelectronic and conductive devices, food ingredients and packaging, biomedicine, and 3D printing technol.
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    23. 23
      Anwar, B.; Bundjali, B.; Arcana, I. M. Isolation of Cellulose Nanocrystals from Bacterial Cellulose Produced from Pineapple Peel Waste Juice as Culture Medium. Procedia Chem. 2015, 16, 279– 284,  DOI: 10.1016/j.proche.2015.12.051
      23
      Isolation of Cellulose Nanocrystals from Bacterial Cellulose Produced from Pineapple Peel Waste Juice as Culture Medium
      Anwar, Budiman; Bundjali, Bunbun; Arcana, I. Made
      Procedia Chemistry (2015), 16 (), 279-284CODEN: PCRHBG; ISSN:1876-6196. (Elsevier B.V.)
      Cellulose nanocrystals (CNC) were isolated by the sulfuric acid hydrolysis of bacterial cellulose (BC) produced by Gluconacetobacter xylinus using pineapple peel waste juice as culture medium. Optimal conditions of the acid hydrolysis were obtained at concn. of sulfuric acid of 50%, hydrolysis time ranging 25∼40 min and temp. at 50 °C. The FTIR study shows that the CNC spectrum were similar with BC which indicated that both have similar chem. compn.; however there are some peaks alteration at 2900 cm-1 and 1430 cm-1 which indicated that BC has changed into CNC. The crystallinity of CNC detd. by FTIR was found to be higher than BC. By TEM observation, the CNC particles had av. length of 325 nm and diam. of 25 nm with av. aspect ratio (L/D) around 13. The TEM images also show the morphol. of CNC that has rod-like structure.
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    24. 24
      Raghav, N.; Sharma, M. R.; Kennedy, J. F. Nanocellulose: A mini-review on types and use in drug delivery systems. Carbohydr. Polym. Technol. Appl. 2021, 2, 100031,  DOI: 10.1016/j.carpta.2020.100031
      24
      Nanocellulose: A mini-review on types and use in drug delivery systems
      Raghav, N.; Sharma, Manishita R.; Kennedy, John F.
      Carbohydrate Polymer Technologies and Applications (2021), 2 (), 100031CODEN: CPTACM; ISSN:2666-8939. (Elsevier Ltd.)
      A review. Development of effective drug delivery systems by the exploitation of biocompatible, inert nanomaterials has become the thrust areas of research in medicinal chem. Out of various materials of significance, one is nanocryst. cellulose due to its biocompatibility and inertness. Further its surface modification can also be accomplished using variety of methods. In the present review we have compiled different types of nanocellulose and their use as drug delivery systems. The review recapitulate the literature not reported in recent reviews of 2019 and 2020. The review is focused on method of prepn. of nanocellulose and its application in oral, transdermal and local drug delivery systems. Limitations and advantages of surface modified nanocellulose is also discussed.
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    25. 25
      Iguchi, M.; Yamanaka, S.; Budhiono, A. Bacterial cellulose─a masterpiece of nature’s arts. J. Mater. Sci. 2000, 35, 261– 270,  DOI: 10.1023/a:1004775229149
      25
      Bacterial cellulose - a masterpiece of Nature's arts
      Iguchi, M.; Yamanaka, S.; Budhiono, A.
      Journal of Materials Science (2000), 35 (2), 261-270CODEN: JMTSAS; ISSN:0022-2461. (Kluwer Academic Publishers)
      A review with 41 refs. Ever since its remarkable mech. properties were found fifteen years ago, interest has grown in bacterial cellulose for which the use had been more or less limited to the manuf. of nata-de-coco, an indigenous food of Southeast Asia. This paper reviews the progress of relevant studies, including the prodn. of cellulose by bacteria, the formation of microfibrils and gel layer, the properties of gel and processed sheets, and some aspects of applications.
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    26. 26
      Fleury, B.; Abraham, E.; De La Cruz, J. A.; Chandrasekar, V. S.; Senyuk, B.; Liu, Q.; Cherpak, V.; Park, S.; ten Hove, J. B.; Smalyukh, I. I. Aerogel from Sustainably Grown Bacterial Cellulose Pellicles as a Thermally Insulative Film for Building Envelopes. ACS Appl. Mater. Interfaces 2020, 12, 34115– 34121,  DOI: 10.1021/acsami.0c08879
      26
      Aerogel from Sustainably Grown Bacterial Cellulose Pellicles as a Thermally Insulative Film for Building Envelopes
      Fleury, Blaise; Abraham, Eldho; De La Cruz, Joshua A.; Chandrasekar, Varun S.; Senyuk, Bohdan; Liu, Qingkun; Cherpak, Vladyslav; Park, Sungoh; ten Hove, Jan Bart; Smalyukh, Ivan I.
      ACS Applied Materials & Interfaces (2020), 12 (30), 34115-34121CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
      Improving building energy performance requires the development of new highly insulative materials. An affordable retrofitting soln. comprising a thin film could improve the resistance to heat flow in both residential and com. buildings and reduce overall energy consumption. Here, we propose cellulose aerogel films formed from pellicles produced by the bacteria Gluconacetobacter hansenii as insulation materials. We studied the impact of the d. and nanostructure on the aerogels' thermal properties. A thermal cond. as low as 13 mW/(K·m) was measured for native pellicle-based aerogels that were dried as-is with minimal post-treatment. The use of waste from the beer brewing industry as a soln. to grow the pellicle maintained the cellulose yield obtained with std. Hestrin-Schramm media, making our product more affordable and sustainable. In the future, our work can be extended through further diversification of food wastes as the substrate sources, facilitating higher potential prodn. and larger applications.
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    27. 27
      Chen, Y.; Zhang, L.; Yang, Y.; Pang, B.; Xu, W.; Duan, G.; Jiang, S.; Zhang, K. Recent Progress on Nanocellulose Aerogels: Preparation, Modification, Composite Fabrication, Applications. Adv. Mater. 2021, 33, 2005569,  DOI: 10.1002/adma.202005569
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      Recent Progress on Nanocellulose Aerogels: Preparation, Modification, Composite Fabrication, Applications
      Chen, Yiming; Zhang, Lin; Yang, Yang; Pang, Bo; Xu, Wenhui; Duan, Gaigai; Jiang, Shaohua; Zhang, Kai
      Advanced Materials (Weinheim, Germany) (2021), 33 (11), 2005569CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)
      A review. The rapid development of modern industry and excessive consumption of petroleum-based polymers have triggered a double crisis presenting a shortage of nonrenewable resources and environmental pollution. However, this has provided an opportunity to stimulate researchers to harness native biobased materials for novel advanced materials and applications. Nanocellulose-based aerogels, using abundant and sustainable cellulose as raw material, present a third-generation of aerogels that combine traditional aerogels with high porosity and large sp. surface area, as well as the excellent properties of cellulose itself. Currently, nanocellulose aerogels provide a highly attention-catching platform for a wide range of functional applications in various fields, e.g., adsorption, sepn., energy storage, thermal insulation, electromagnetic interference shielding, and biomedical applications. Here, the prepn. methods, modification strategies, composite fabrications, and further applications of nanocellulose aerogels are summarized, with addnl. discussions regarding the prospects and potential challenges in future development.
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    28. 28
      Huang, Y.; Huang, X.; Ma, M.; Hu, C.; Seidi, F.; Yin, S.; Xiao, H. Recent advances on the bacterial cellulose-derived carbon aerogels. J. Mater. Chem. C 2021, 9, 818– 828,  DOI: 10.1039/d0tc05433j
      28
      Recent advances on the bacterial cellulose-derived carbon aerogels
      Huang, Yang; Huang, Xiangzhou; Ma, Mengtao; Hu, Chenyao; Seidi, Farzad; Yin, Sha; Xiao, Huining
      Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2021), 9 (3), 818-828CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
      A review. Bacterial cellulose (BC), sustainable biomass, has long been envisioned as a fantastic biomass material since it was discovered by Brown in 1886. BC cultivated in static medium appears as a never-dried hydrogel, wherein numerous nanofibers are highly interconnected, building into a three-dimensional (3D) architecture. Although BC has achieved great success in the area of biol. medicine, the electronic inertness and susceptible bio-invasion restrict its further applications demanding electronic migration and durability. Carbonization has been employed to endow BC with superior cond. and chem. tolerance without destroying the 3D architecture. Moreover, carbonized BC (CBC) exhibits exceptional properties such as ultralightweight, high surface area, good volumetric resilience, and superhydrophobicity, which are necessary for electrochem. energy, microwave attenuation, and selective absorption. The industrial prodn. of BC facilitates the massive fabrication of high value-added CBC with low-cost precursors. This review summarizes the latest developments on the CBC-based functional materials, including state-of-the-art design concepts and synthetic strategies. Our prospects on the major obstacles in the approach of further exploitation of CBC, as well as the promising avenues in front of these issues are proposed in this review.
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    29. 29
      Pham, T. T.; Tran, T. T. A. Evaluation of the crystallinity of bacterial cellulose produced from pineapple waste solution by using acetobacter xylinum. ASEAN Eng. J. 2023, 13, 81– 91,  DOI: 10.11113/aej.v13.18868
      There is no corresponding record for this reference.
    30. 30
      Feng, J.; Nguyen, S. T.; Fan, Z.; Duong, H. M. Advanced fabrication and oil absorption properties of super-hydrophobic recycled cellulose aerogels. Chem. Eng. J. 2015, 270, 168– 175,  DOI: 10.1016/j.cej.2015.02.034
      30
      Advanced fabrication and oil absorption properties of super-hydrophobic recycled cellulose aerogels
      Feng, Jingduo; Nguyen, Son T.; Fan, Zeng; Duong, Hai M.
      Chemical Engineering Journal (Amsterdam, Netherlands) (2015), 270 (), 168-175CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
      A facile and cost-effective synthesis method of biocompatible cellulose aerogels using recycled cellulose fibers of paper waste and Kymene crosslinker is successfully developed for the first time. After coated with methyltrimethoxysilane (MTMS) via chem. vapor deposition, the recycled cellulose aerogels yields very stable super-hydrophobicity for over five months and excellent oil absorption capacities of up to 95 g g-1 with the 0.25 wt.% cellulose aerogel. Effects of different cellulose fiber concns., different ratios of the cellulose and Kymene crosslinker compn., ambient temps. and pH values of the environment on the oil absorption behavior of the cellulose aerogels are also quantified comprehensively. The exptl. results show the cellulose aerogels yield the max. absorption capacity at 50 °C. Compared to the pseudo first-order model, the pseudo second-order model is more validated for the oil absorption kinetics study. The recycled cellulose aerogels are promising for replacing earth-unfriendly polymer-based oil sorbents due to their high oil absorption capacities.
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    31. 31
      Eichhorn, S. J.; Sampson, W. W. Relationships between specific surface area and pore size in electrospun polymer fibre networks. J. R. Soc., Interface 2010, 7, 641– 649,  DOI: 10.1098/rsif.2009.0374
      31
      Relationships between specific surface area and pore size in electrospun polymer fibre networks
      Eichhorn, S. J.; Sampson, W. W.
      Journal of the Royal Society, Interface (2010), 7 (45), 641-649CODEN: JRSICU; ISSN:1742-5689. (Royal Society)
      From consideration of the extent of contact between fibers in electrospun polymer networks, we provide theory relating the sp. surface area of the network to the characteristic dimensions of interfiber voids. We show that these properties are strongly influenced by the cross-sectional morphologies of fibers. Whereas porosity has a strong influence on pore dimensions, in the range of porosities typically obtained in real networks, its influence on sp. surface area is weak. By considering ref. geometries of collapsed ribbons and fibers with circular cross sections, we demonstrate that at a given network porosity, fiber parameters that increase the sp. surface area reduce the characteristic dimensions of voids. The implications of the theory, mainly in the context of cell proliferation on electrospun polymer scaffolds, are discussed; the theory has relevance also to future applications of these materials in composites.
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    32. 32
      Cervin, N. T.; Aulin, C.; Larsson, P. T.; Wågberg, L. Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids. Cellulose 2012, 19, 401– 410,  DOI: 10.1007/s10570-011-9629-5
      32
      Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids
      Cervin, Nicholas Tchang; Aulin, Christian; Larsson, Per Tomas; Waagberg, Lars
      Cellulose (Dordrecht, Netherlands) (2012), 19 (2), 401-410CODEN: CELLE8; ISSN:0969-0239. (Springer)
      A novel type of sponge-like material for the sepn. of mixed oil and water liqs. has been prepd. by the vapor deposition of hydrophobic silanes on ultra-porous nanocellulose aerogels. To achieve this, a highly porous (>99%) nanocellulose aerogel with high structural flexibility and robustness is first formed by freeze-drying an aq. dispersion of the nanocellulose. The d., pore size distribution and wetting properties of the aerogel can be tuned by selecting the concn. of the nanocellulose dispersion before freeze-drying. The hydrophobic light- wt. aerogels are almost instantly filled with the oil phase when selectively absorbing oil from water, with a capacity to absorb up to 45 times their own wt. in oil. The oil can also be drained from the aerogel and the aerogel can then be reused for a second absorption cycle.
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    33. 33
      Revellame, E. D.; Fortela, D. L.; Sharp, W.; Hernandez, R.; Zappi, M. E. Adsorption kinetic modeling using pseudo-first order and pseudo-second order rate laws: A review. Clean. Eng. and Technol. 2020, 1, 100032,  DOI: 10.1016/j.clet.2020.100032
      There is no corresponding record for this reference.
    34. 34
      Kalam, S.; Abu-Khamsin, S. A.; Kamal, M. S.; Patil, S. Surfactant Adsorption Isotherms: A Review. ACS Omega 2021, 6, 32342– 32348,  DOI: 10.1021/acsomega.1c04661
      34
      Surfactant Adsorption Isotherms: A Review
      Kalam, Shams; Abu-Khamsin, Sidqi A.; Kamal, Muhammad Shahzad; Patil, Shirish
      ACS Omega (2021), 6 (48), 32342-32348CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      A review. The need to minimize surfactant adsorption on rock surfaces has been a challenge for surfactant-based, chem.-enhanced oil recovery (cEOR) techniques. Modeling of adsorption exptl. data is very useful in estg. the extent of adsorption and, hence, optimizing the process. This paper presents a mini-review of surfactant adsorption isotherms, focusing on theories of adsorption and the most frequently used adsorption isotherm models. Two-step and four-region adsorption theories are well-known, with the former representing adsorption in two steps, while the latter distinguishes four regions in the adsorption isotherm. Langmuir and Freundlich are two-parameter adsorption isotherms that are widely used in cEOR studies. The Langmuir isotherm is applied to monolayer adsorption on homogeneous sites, whereas the Freundlich isotherm suites are applied to multilayer adsorption on heterogeneous sites. Some more complex adsorption isotherms are also discussed in this paper, such as Redlich-Peterson and Sips isotherms, both involve three parameters. This paper will help select and apply a suitable adsorption isotherm to exptl. data.
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    35. 35
      Mullet, M.; Fievet, P.; Szymczyk, A.; Foissy, A.; Reggiani, J. C.; Pagetti, J. A simple and accurate determination of the point of zero charge of ceramic membranes. Desalination 1999, 121, 41– 48,  DOI: 10.1016/s0011-9164(99)00006-5
      35
      A simple and accurate determination of the point of zero charge of ceramic membranes
      Mullet, M.; Fievet, P.; Szymczyk, A.; Foissy, A.; Reggiani, J.-C.; Pagetti, J.
      Desalination (1999), 121 (1), 41-48CODEN: DSLNAH; ISSN:0011-9164. (Elsevier Science B.V.)
      A simple, accurate detn. of the point of zero charge (PZC) of a ceramic membrane is reported, based on pH variation measurements on adding an amphoteric oxide in a soln. of a given pH. Up to now, this method was effective for studying powder dispersions; in this work it was extended to ceramic membranes. An exptl. set-up that allows the performance of pH measurements on a soln. continuously circulating through the membrane is discussed. It verified that the PZC, detd. in presence of an indifferent electrolyte, is the same as the isoelec. point (or PZC) detd. with std. electrokinetic methods. The shift in the PZC towards a higher and lower pH, in presence of Na2SO4 and CaCl2 solns., resp., confirmed the specific adsorption of SO42- and Ca2+ ions and validated the method used. This method was compared with the known salt addn. method, conducted on the crushed membrane. This led to a different PZC value, demonstrating the importance of performing measurements directly on membranes themselves. Another interesting aspect in the method presented is that it permits direct assessment of the abs. value of the surface charge d. of the membrane. Results obtained were in good agreement with data reported in the literature on mineral oxides.
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    36. 36
      Abral, H.; Lawrensius, V.; Handayani, D.; Sugiarti, E. Preparation of nano-sized particles from bacterial cellulose using ultrasonication and their characterization. Carbohydr. Polym. 2018, 191, 161– 167,  DOI: 10.1016/j.carbpol.2018.03.026
      36
      Preparation of nano-sized particles from bacterial cellulose using ultrasonication and their characterization
      Abral, Hairul; Lawrensius, Vincent; Handayani, Dian; Sugiarti, Eni
      Carbohydrate Polymers (2018), 191 (), 161-167CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
      As more applications for nano-sized natural particles are discovered, simple, environmentally friendly ways to produce these particles become more important. This work preps. and characterizes nano-size bacterial cellulose particles using ultrasonication. Pellicle from nata de coco contg. nanofibers was broken up in an elec. blender, then sonicated using an ultrasonic probe at 20kHz and 3W/mL for 30, 60 and 90 min. Transmission electron microscope observations indicate the particles become nano-sized after 60 min ultrasound. The max. decompn. temp. before sonication was 373°, decreased to 357° after 60 min ultrasonication. Moisture absorption of the 90 min sonicated particles film is 60% slower compared to non-sonicated particles. After ultrasonication, the crystallinity index of the cellulose decreases. The functional groups of non-sonicated and sonicated cellulose remain the same. This study promotes a potential method of fabrication of nano-sized particles from pure bacterial cellulose.
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    37. 37
      Li, Z.; Zhong, L.; Zhang, T.; Qiu, F.; Yue, X.; Yang, D. Sustainable, Flexible, and Superhydrophobic Functionalized Cellulose Aerogel for Selective and Versatile Oil/Water Separation. ACS Sustain. Chem. Eng. 2019, 7, 9984– 9994,  DOI: 10.1021/acssuschemeng.9b01122
      37
      Sustainable, Flexible, and Superhydrophobic Functionalized Cellulose Aerogel for Selective and Versatile Oil/Water Separation
      Li, Zhangdi; Zhong, Li; Zhang, Tao; Qiu, Fengxian; Yue, Xuejie; Yang, Dongya
      ACS Sustainable Chemistry & Engineering (2019), 7 (11), 9984-9994CODEN: ASCECG; ISSN:2168-0485. (American Chemical Society)
      Aerogels, as ultralight three-dimensional (3D) highly porous materials, show great superiority in oil and org. pollutant cleanup. Notably, biomass aerogels have also attracted wide interest due to the advantages of huge reserves, low cost, renewability, biodegrdn., and nontoxicity to the environment. Herein, a sustainable, flexible, and superhydrophobic functionalized cellulose aerogel, copper nanoparticles-coated cellulose aerogel (Cu/CEA), is reported. The hydrophobic Cu/CEA was simply fabricated by one-step depositing Cu nanoparticles coating on the cellulose fibers extd. from renewable natural sisal in liq. phase followed by freeze-drying. The hydrophobic functionalization approach is facile, cost-effective, and suitable for large-scale prodn. and environmental friendliness, without addnl. org. hydrophobic modification. The highly porous Cu/CEA as absorbent can selectively and quickly collect oily contaminant, exhibiting high oil absorption capacity and rate, and good recyclability. In addn., it can also act as a thick film to continuously and rapidly sep. oil/water mixts. including emulsions, possessing very high sepn. efficiency and flow rate. Hence, the versatile and high-performance functionalized cellulose aerogel possesses a promising practical application in oily wastewater treatment and pollution remediation.
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    38. 38
      Mohamed, M. A.; Abd Mutalib, M.; Mohd Hir, Z. A.; M Zain, M.; Mohamad, A. B.; Jeffery Minggu, L.; Awang, N. A.; Salleh, W.; Salleh, W. N. An overview on cellulose-based material in tailoring bio-hybrid nanostructured photocatalysts for water treatment and renewable energy applications. Int. J. Biol. Macromol. 2017, 103, 1232– 1256,  DOI: 10.1016/j.ijbiomac.2017.05.181
      38
      An overview on cellulose-based material in tailoring bio-hybrid nanostructured photocatalysts for water treatment and renewable energy applications
      Mohamed, Mohamad Azuwa; Abd Mutalib, Muhazri; Mohd. Hir, Zul Adlan; Zain, M. F. M.; Mohamad, Abu Bakar; Minggu, Lorna Jeffery; Awang, Nor Asikin; Salleh, W. N. W.
      International Journal of Biological Macromolecules (2017), 103 (), 1232-1256CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      A review. A combination between the nanostructured photocatalyst and cellulose-based materials promotes a new functionality of cellulose towards the development of new bio-hybrid materials for various applications esp. in water treatment and renewable energy. The excellent compatibility and assocn. between nanostructured photocatalyst and cellulose-based materials was induced by bio-combability and high hydrophilicity of the cellulose components. The electron rich hydroxyl group of celluloses helps to promote superior interaction with photocatalyst. The formation of bio-hybrid nanostructured are attaining huge interest nowadays due to the synergistic properties of individual cellulose-based material and photocatalyst nanoparticles. Therefore, in this review we introduce some cellulose-based material and discusses its compatibility with nanostructured photocatalyst in terms of phys. and chem. properties. In addn., we gather information and evidence on the fabrication techniques of cellulose-based hybrid nanostructured photocatalyst and its recent application in the field of water treatment and renewable energy.
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    39. 39
      Mohamad, S.; Abdullah, L. C.; Jamari, S. S.; Al Edrus, S. S. O.; Aung, M. M.; Mohamad, S. F. S. Influence of drying method on the crystal structure and thermal property of oil palm frond juice-based bacterial cellulose. J. Mater. Sci. 2022, 57, 1462– 1473,  DOI: 10.1007/s10853-021-06685-5
      39
      Influence of drying method on the crystal structure and thermal property of oil palm frond juice-based bacterial cellulose
      Mohamad, Shahril; Abdullah, Luqman Chuah; Jamari, Saidatul Shima; Al Edrus, Syeed Saifulazry Osman; Aung, Min Min; Mohamad, Sharifah Fathiyah Sy
      Journal of Materials Science (2022), 57 (2), 1462-1473CODEN: JMTSAS; ISSN:0022-2461. (Springer)
      Dehydration of wet bacterial cellulose (BC) mainly focuses on the phys. characteristic or mech. strength, but its polymorph crystal structure and thermal properties were rarely discussed. Herein, this study utilizes the drying method of hot-pressed and freeze-dried to the wet BC to elucidate the BC polymorph crystal structure in correlation with the BC crystallinity and thermal properties. The results indicate that dehydration of BC using hot-pressed (BC-HP) method reduced the cellulose Iα allomorph fraction by ± 5.0%, increased the crystallinity by ± 5.0%, but lower in thermal stability compared to freeze-dried (BC-FD) method. Addnl., BC-HP shows an exothermic reaction of melting at lower enthalpy value which is contradict to BC-FD and plant cellulose that presented an endothermic reaction with higher enthalpy values. Thus, investigation on BC polymorph crystal structure and thermal properties may offer an important role to regulate the desired characteristic of the dried BC.
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    40. 40
      Illa, M. P.; Sharma, C. S.; Khandelwal, M. Tuning the physiochemical properties of bacterial cellulose: effect of drying conditions. J. Mater. Sci. 2019, 54, 12024– 12035,  DOI: 10.1007/s10853-019-03737-9
      40
      Tuning the physiochemical properties of bacterial cellulose: effect of drying conditions
      Illa, Mani Pujitha; Sharma, Chandra S.; Khandelwal, Mudrika
      Journal of Materials Science (2019), 54 (18), 12024-12035CODEN: JMTSAS; ISSN:0022-2461. (Springer)
      Bacteria have an ability to produce cellulose in pure form without any impurities such as hemicellulose and lignin, unlike plant cellulose. Bacterial cellulose as-produced with 3-D interwoven nanofibrous network is superior to plant cellulose in terms of mech. properties, porosity, crystallinity, water holding capacity, and sustainability. In its natural form, bacterial cellulose is in the form of a hydrogel, which implies high porosity and holding capacity, however, to use it for different applications, water needs to be removed. The phys. properties of bacterial cellulose such as morphol., porosity, and mech. strength are vastly affected by the drying method employed. This paper presents a case study in which we produced bacterial cellulose using two different strains, followed by systematically studying the effect of drying (oven and freeze drying) on physiochem., morphol., and structural properties of as-produced bacterial cellulose using Fourier transform IR spectroscopy, X-ray diffraction, field emission SEM, BET surface area, and tensile testing. Oven-dried bacterial cellulose showed higher crystallinity, reduced fiber diam., and narrow size distribution and higher mech. properties as compared to freeze-dried bacterial cellulose. Understanding so developed in this work may allow us to simply tune the bacterial cellulose properties for a given application.
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    41. 41
      Ul-Islam, M.; Khattak, W. A.; Kang, M.; Kim, S. M.; Khan, T.; Park, J. K. Effect of post-synthetic processing conditions on structural variations and applications of bacterial cellulose. Cellulose 2013, 20, 253– 263,  DOI: 10.1007/s10570-012-9799-9
      41
      Effect of post-synthetic processing conditions on structural variations and applications of bacterial cellulose
      Ul-Islam, Mazhar; Khattak, Waleed Ahmad; Kang, Minkyung; Kim, Sang Min; Khan, Taous; Park, Joong Kon
      Cellulose (Dordrecht, Netherlands) (2013), 20 (1), 253-263CODEN: CELLE8; ISSN:0969-0239. (Springer)
      Physicochem. properties of materials can be amended by altering their phys. structure through different processing conditions. The present study was conducted to investigate the post-synthesis structural variations and physico-mech. properties of bacterial cellulose (BC) sheets prepd. using different drying methods. Wet BC sheets of the same origin were freeze dried (BC-FD), dried at room temp. (25 °C) (BC-DRT), and dried at elevated temp. (50 °C) (BC-DHT). FE-SEM micrographs revealed that BC-DRT and BC-DHT had a more tightly packed and compact structure than the loosely held fibrils of BC-FD. XRD anal. revealed the relative crystallinity of the BC sample to be 64.60, 59.16, and 47.20 % for BC-DHT, BC-DRT and BC-FD, resp. The water holding capacity (WHC) of the BC-FD was higher than that of the other two samples. Four consecutive drying and rewetting cycles demonstrated that the WHC of all samples decreased with each cycle. The WHC of BC-DRT and BC-DHT was reduced to almost 0 after the first drying cycle, but the BC-FD samples were able to regain some of their WHC. The tensile strength and elongation modulus were in the order of BC-DHT > BC-DRT > BC-FD. Overall, the results of this study revealed that the post-synthetic processing conditions had a strong effect on the structure and physico-mech. properties of BC.
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    42. 42
      Zhang, C. J.; Wang, L.; Zhao, J. C.; Zhu, P. Effect of Drying Methods on Structure and Mechanical Properties of Bacterial Cellulose Films. Adv. Mater. Res. 2011, 239–242, 2667– 2670,  DOI: 10.4028/www.scientific.net/amr.239-242.2667
      42
      Effect of drying methods on structure and mechanical properties of bacterial cellulose films
      Zhang, Chuanjie; Wang, Liu; Zhao, Jinchao; Zhu, Ping
      Advanced Materials Research (Durnten-Zurich, Switzerland) (2011), 239-242 (Pt. 4, Advanced Materials), 2667-2670CODEN: AMREFI; ISSN:1022-6680. (Trans Tech Publications Ltd.)
      Bacterial cellulose (BC) gelatinous films prepd. in stationary culture were dried by three different drying methods: hot air drying, vacuum drying and vacuum freezing drying. The structure of dried bacterial cellulose films was characterized using SEM, IR spectroscopy and X-ray diffraction (XRD), and mech. properties were tested. The results showed that the surface of films prepd. by hot air drying were uniform and dense, cavities and cracks configurations existed in vacuum dried films, and layer and porous structures were obsd. in vacuum freezing dried films. FTIR spectra and X-ray pattern confirmed that vacuum freezing drying reduced the strength of hydrogen bonds between cellulose macromols. and the degree of crystallinity of BC films but had little influence on the crystal structure. For those reasons, mech. properties of BC films prepd. by vacuum freezing drying were lower than that of those films by other methods.
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    43. 43
      Zimmermann, M. V. G.; Borsoi, C.; Lavoratti, A.; Zanini, M.; Zattera, A. J.; Santana, R. M. C. Drying techniques applied to cellulose nanofibers. J. Reinf. Plast. Compos. 2016, 35, 682– 697,  DOI: 10.1177/0731684415626286
      43
      Drying techniques applied to cellulose nanofibers
      Zimmermann, Matheus V. G.; Borsoi, Cleide; Lavoratti, Alessandra; Zanini, Marcia; Zattera, Ademir J.; Santana, Ruth M. C.
      Journal of Reinforced Plastics and Composites (2016), 35 (8), 682-697CODEN: JRPCDW; ISSN:0731-6844. (Sage Publications Ltd.)
      A review. Nanotechnol. applied to cellulosic fibers has quickly become an interdisciplinary field with great interest in the application as reinforcement in polymer composites, mainly due to the abundance of these raw materials, and to their mech. properties and multifunctionality. However, one of the crit. points to obtain individualized cellulose nanofibers is the drying technique (dehydration), since most of the nanofiber processes are performed in the liq. phase. According to the methodol. applied to the cellulose water dehydration process, various morphologies and properties can be obtained in the cellulose fibers. This review study aims to discuss the main processes used to obtain nanocellulose (chem. and mech.) and the drying techniques applied to nanocellulose structures, such as conventional oven drying, freeze drying (lyophilization), supercrit. extn., and spray drying.
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    44. 44
      Liebner, F.; Potthast, A.; Rosenau, T.; Haimer, E.; Wendland, M. Cellulose aerogels: Highly porous, ultra-lightweight materials. Holzforschung 2008, 62, 129– 135,  DOI: 10.1515/hf.2008.051
      44
      Cellulose aerogels: highly porous, ultra-lightweight materials
      Liebner, Falk; Potthast, Antje; Rosenau, Thomas; Haimer, Emmerich; Wendland, Martin
      Holzforschung (2008), 62 (2), 129-135CODEN: HOLZAZ; ISSN:0018-3830. (Walter de Gruyter GmbH & Co. KG)
      Cellulosic aerogels are intriguing new materials produced by supercrit. drying of regenerated cellulose obtained by solvent exchange of solid Lyocell moldings. From N-methylmorpholine-N-oxide (NMMO) solns. with cellulose contents between 1 and 12%, dimensionally stable cellulose bodies are produced, in which the soln. structure of the cellulose is largely preserved and transferred into the solid state, the material having densities down to 0.05 g cm-3 and surface areas of up to 280 m2 g-1. In this study, several aspects of cellulosic aerogel prodn. are communicated: the stabilization of the cellulose solns. against degrdn. reactions by agents suitable for later extn. and drying, a reliable extn. and drying procedure by supercrit. carbon dioxide, the advantages of DMSO/NMMO in this procedure as a solvent/non-solvent pair, and some data on the phys. properties of the materials.
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    45. 45
      Liebner, F.; Haimer, E.; Potthast, A.; Loidl, D.; Tschegg, S.; Neouze, M.-A.; Wendland, M.; Rosenau, T. Cellulosic aerogels as ultra-lightweight materials. Part 2: Synthesis and properties 2nd ICC 2007, Tokyo, Japan, October 25–29, 2007. Holzforschung 2009, 63, 3– 11,  DOI: 10.1515/hf.2009.002
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      Cellulosic aerogels as ultra-lightweight materials. Part 2: synthesis and properties
      Liebner, Falk; Haimer, Emmerich; Potthast, Antje; Loidl, Dieter; Tschegg, Stefanie; Neouze, Marie-Alexandra; Wendland, Martin; Rosenau, Thomas
      Holzforschung (2009), 63 (1), 3-11CODEN: HOLZAZ; ISSN:0018-3830. (Walter de Gruyter GmbH & Co. KG)
      Ultra-lightwt. cellulose aerogels can be obtained in three steps: (1) prepn. of a cellulose soln. in molten N-methylmorpholine-N-oxide monohydrate (NMMO·H2O) at 110-120°C and casting of the viscous mass into molds; (2) extn. of the solidified castings with ethanol to initiate cellulose aggregation and to remove NMMO·H2O so that the fragile, fine-porous texture of cellulose II is largely retained; and (3) drying of the lyogel using supercrit. carbon dioxide (scCO2). According to this approach, cellulosic aerogels were prepd. from eight com. cellulosic materials and pulps and analyzed for selected chem., physicochem. and mech. parameters. The results reveal that all aerogels obtained from 3% cellulose contg. NMMO·H2O melts had a largely uniform mesoporous structure with an av. pore size of ∼9-12 nm, surface area of 190-310 m2 g-1, and specific d. of 0.046-0.069 g cm-3, but rather low mech. stability expressed as compressive yield strain of 2.9-5.5%. All samples showed viscoelastic behavior, with Young's modulus ranging from ∼5 to 10 N mm-2. Doubling the cellulose content in the NMMO·H2O melt from 3% to 6% increased Young's modulus by one order of magnitude. Shrinkage of the fragile cellulose bodies during scCO2 drying was still considerable and is subject to further investigations. Influencing parameters such as scCO2 pressure, cellulose content, regenerating solvent and the no. of regenerating baths were optimized.
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    46. 46
      Liebner, F.; Haimer, E.; Wendland, M.; Neouze, M. A.; Schlufter, K.; Miethe, P.; Heinze, T.; Potthast, A.; Rosenau, T. Aerogels from unaltered bacterial cellulose: application of scCO2 drying for the preparation of shaped, ultra-lightweight cellulosic aerogels. Macromol. Biosci. 2010, 10, 349– 352,  DOI: 10.1002/mabi.200900371
      46
      Aerogels from Unaltered Bacterial Cellulose: application of scCO2 Drying for the Preparation of Shaped, Ultra-Lightweight Cellulosic Aerogels
      Liebner, Falk; Haimer, Emmerich; Wendland, Martin; Neouze, Marie-Alexandra; Schlufter, Kerstin; Miethe, Peter; Heinze, Thomas; Potthast, Antje; Rosenau, Thomas
      Macromolecular Bioscience (2010), 10 (4), 349-352CODEN: MBAIBU; ISSN:1616-5187. (Wiley-VCH Verlag GmbH & Co. KGaA)
      Bacterial cellulose produced by the gram-neg. bacterium Gluconacetobacter xylinum was found to be an excellent native starting material for prepg. shaped ultra-lightwt. cellulose aerogels. The procedure comprises thorough washing and sterilization of the aquogel, quant. solvent exchange and subsequent drying with supercrit. carbon dioxide at 40° and 100 bar. The av. d. of the obtained dry cellulose aerogels is only about 8 mg/cm-3 which is comparable to the most lightwt. silica aerogels and distinctly lower than all values for cellulosic aerogels obtained from plant cellulose so far. SEM, ESEM, and nitrogen adsorption expts. at 77 K reveal an open-porous network structure that consists of a comparatively high percentage of large mesopores and smaller macropores.
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    47. 47
      Chang, S. S.; Clair, B.; Ruelle, J.; Beauchene, J.; Di Renzo, F.; Quignard, F.; Zhao, G. J.; Yamamoto, H.; Gril, J. Mesoporosity as a new parameter for understanding tension stress generation in trees. J. Exp. Bot. 2009, 60, 3023– 3030,  DOI: 10.1093/jxb/erp133
      47
      Mesoporosity as a new parameter for understanding tension stress generation in trees
      Chang, Shan-Shan; Clair, Bruno; Ruelle, Julien; Beauchene, Jacques; Di Renzo, Francesco; Quignard, Francoise; Zhao, Guang-Jie; Yamamoto, Hiroyuki; Gril, Joseph
      Journal of Experimental Botany (2009), 60 (11), 3023-3030CODEN: JEBOA6; ISSN:0022-0957. (Oxford University Press)
      The mechanism for tree orientation in angiosperms is based on the prodn. of high tensile stress on the upper side of the inclined axis. In many species, the stress level is strongly related to the presence of a peculiar layer, called the G-layer, in the fiber cell wall. The structure of the G-layer has recently been described as a hydrogel thanks to N2 adsorption-desorption isotherms of supercritically dried samples showing a high mesoporosity (pores size from 2-50 nm). This led us to revisit the concept of the G-layer that had been, until now, only described from anatomical observation. Adsorption isotherms of both normal wood and tension wood have been measured on six tropical species. Measurements show that mesoporosity is high in tension wood with a typical thick G-layer while it is much less with a thinner G-layer, sometimes no more than normal wood. The mesoporosity of tension wood species without a G-layer is as low as in normal wood. Not depending on the amt. of pores, the pore size distribution is always centered around 6-12 nm. These results suggest that, among species producing fibers with a G-layer, large structural differences of the G-layer exist between species.
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    48. 48
      Guo, J.; Catchmark, J. M. Surface area and porosity of acid hydrolyzed cellulose nanowhiskers and cellulose produced by Gluconacetobacter xylinus. Carbohydr. Polym. 2012, 87, 1026– 1037,  DOI: 10.1016/j.carbpol.2011.07.060
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      Surface area and porosity of acid hydrolyzed cellulose nanowhiskers and cellulose produced by Gluconacetobacter xylinus
      Guo, Jing; Catchmark, Jeffrey M.
      Carbohydrate Polymers (2012), 87 (2), 1026-1037CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
      The phys. parameters of cellulose such as surface area and porosity are important in the development of cellulose composites which may contain valuable additives which bind to cellulose. In this area, the use of acid hydrolyzed nano-dimensional cellulose nanowhiskers (CNWs) has attracted significant interest, yet the surface area and porosity of these materials have not been explored exptl. The objective of this work was to characterize the surface area and porosity of CNWs from different origins (plant cotton/bacterium Gluconacetobacter xylinus) and different acid treatments (H2SO4/HCl) by N2 adsorption; as well as to compare surface area and porosity of bacterial cellulose synthesized by static and agitated cultures. Our results showed that CNWs produced from H2SO4/HCl exhibited significantly increased surface area and porosity relative to starting material cotton fiber CF11. Micropores were generated in HCl hydrolyzed CNWs but not in H2SO4 hydrolyzed CNWs. Bacterial CNWs exhibited larger surface area and porosity compared to plant CNWs. Cellulose synthesized by G. xylinus ATCC 700178 from agitated cultures also exhibited less surface area and porosity than those from static cultures.
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    49. 49
      Horvat, G.; Pantic, M.; Knez, Z.; Novak, Z. A Brief Evaluation of Pore Structure Determination for Bioaerogels. Gels 2022, 8, 438,  DOI: 10.3390/gels8070438
      49
      A Brief Evaluation of Pore Structure Determination for Bioaerogels
      Horvat, Gabrijela; Pantic, Milica; Knez, Zeljko; Novak, Zoran
      Gels (2022), 8 (7), 438CODEN: GELSAZ; ISSN:2310-2861. (MDPI AG)
      A review. This review discusses the most commonly employed methods for detg. pore size and pore size distribution in bioaerogels. Aerogels are materials with high porosity and large surface areas. Most of their pores are in the range of mesopores, between 2 and 50 nm. They often have smaller or larger pores, which presents a significant challenge in detg. the exact mean pore size and pore size distribution in such materials. The precision and actual value of the pore size are of considerable importance since pore size and pore size distribution are among the main properties of aerogels and are often directly connected with the final application of those materials. However, many recently published papers discuss or present pore size as one of the essential achievements despite the misinterpretation or the wrong assignments of pore size detn. This review will help future research and publications evaluate the pore size of aerogels more precisely and discuss it correctly. The study covers methods such as gas adsorption, from which BJH and DFT models are often used, SEM, mercury porosimetry, and thermoporometry. The methods are described, and the results obtained are discussed. The following paper shows that there is still no precise method for detg. pore size distribution or mean pore size in aerogels until now. Knowing that, it is expected that this field will evolve in the future.
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    50. 50
      Mi, Q.-y.; Ma, S.-r.; Yu, J.; He, J.-s.; Zhang, J. Flexible and Transparent Cellulose Aerogels with Uniform Nanoporous Structure by a Controlled Regeneration Process. ACS Sustain. Chem. Eng. 2016, 4, 656– 660,  DOI: 10.1021/acssuschemeng.5b01079
      There is no corresponding record for this reference.
    51. 51
      Dos Santos Silva, L.; De Oliveira Carvalho, J.; De Sousa Bezerra, R. D.; Da Silva, M. S.; Ferreira, F. J.; Osajima, J. A.; Da Silva Filho, E. C. Potential of Cellulose Functionalized with Carboxylic Acid as Biosorbent for the Removal of Cationic Dyes in Aqueous Solution. Molecules 2018, 23, 743,  DOI: 10.3390/molecules23040743
      There is no corresponding record for this reference.
    52. 52
      Lahiri, D.; Nag, M.; Dutta, B.; Dey, A.; Sarkar, T.; Pati, S.; Edinur, H. A.; Abdul Kari, Z.; Mohd Noor, N. H.; Ray, R. R. Bacterial Cellulose: Production, Characterization, and Application as Antimicrobial Agent. Int. J. Mol. Sci. 2021, 22, 12984,  DOI: 10.3390/ijms222312984
      52
      Bacterial Cellulose: Production, Characterization, and Application as Antimicrobial Agent
      Lahiri, Dibyajit; Nag, Moupriya; Dutta, Bandita; Dey, Ankita; Sarkar, Tanmay; Pati, Siddhartha; Edinur, Hisham Atan; Abdul Kari, Zulhisyam; Mohd Noor, Noor Haslina; Ray, Rina Rani
      International Journal of Molecular Sciences (2021), 22 (23), 12984CODEN: IJMCFK; ISSN:1422-0067. (MDPI AG)
      A review. Bacterial cellulose (BC) is recognized as a multifaceted, versatile biomaterial with abundant applications. Groups of microorganisms such as bacteria are accountable for BC synthesis through static or agitated fermn. processes in the presence of competent media. In comparison to static cultivation, agitated cultivation provides the max. yield of the BC. A pure cellulose BC can pos. interact with hydrophilic or hydrophobic biopolymers while being used in the biomedical domain. From the last two decades, the reinforcement of biopolymer-based biocomposites and its applicability with BC have increased in the research field. The harmony of hydrophobic biopolymers can be reduced due to the high moisture content of BC in comparison to hydrophilic biopolymers. Mech. properties are the important parameters not only in producing green composite but also in dealing with tissue engineering, medical implants, and biofilm. The wide requisition of BC in medical as well as industrial fields has warranted the scaling up of the prodn. of BC with added economy. This review provides a detailed overview of the prodn. and properties of BC and several parameters affecting the prodn. of BC and its biocomposites, elucidating their antimicrobial and antibiofilm efficacy with an insight to highlight their therapeutic potential.
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    53. 53
      Yang, H.; Yan, R.; Chen, H.; Lee, D. H.; Zheng, C. Characteristics of hemicellulose, cellulose and lignin pyrolysis. Fuel 2007, 86, 1781– 1788,  DOI: 10.1016/j.fuel.2006.12.013
      53
      Characteristics of hemicellulose, cellulose and lignin pyrolysis
      Yang, Haiping; Yan, Rong; Chen, Hanping; Lee, Dong Ho; Zheng, Chuguang
      Fuel (2007), 86 (12-13), 1781-1788CODEN: FUELAC; ISSN:0016-2361. (Elsevier Ltd.)
      The pyrolysis characteristics of three main components (hemicellulose, cellulose and lignin) of biomass were investigated using, resp., a thermogravimetric analyzer (TGA) with differential scanning calorimetry (DSC) detector and a pack bed. The releasing of main gas products from biomass pyrolysis in TGA was online measured using Fourier transform IR (FTIR) spectroscopy. In thermal anal., the pyrolysis of hemicellulose and cellulose occurred quickly, with the wt. loss of hemicellulose mainly happened at 220-315° and that of cellulose at 315-400°. However, lignin was more difficult to decomp., as its wt. loss happened in a wide temp. range (from 160 to 900°) and the generated solid residue was high (∼40%). From the viewpoint of energy consumption in the course of pyrolysis, cellulose behaved differently from hemicellulose and lignin; the pyrolysis of the former was endothermic while that of the latter was exothermic. The main gas products from pyrolyzing the three components were similar, including CO2, CO, CH4 and some orgs. The releasing behaviors of H2 and the total gas yield were measured using Micro-GC when pyrolyzing the three components in a packed bed. Hemicellulose had higher CO2 yield, cellulose generated higher CO yield, and lignin owned higher H2 and CH4 yield. A better understanding to the gas products releasing from biomass pyrolysis could be achieved based on this in-depth investigation on three main biomass components.
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    54. 54
      Eltaweil, A. S.; Elgarhy, G. S.; El-Subruiti, G. M.; Omer, A. M. Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads for efficient adsorption of cationic methylene blue dye. Int. J. Biol. Macromol. 2020, 154, 307– 318,  DOI: 10.1016/j.ijbiomac.2020.03.122
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      Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads for efficient adsorption of cationic methylene blue dye
      Eltaweil, Abdelazeem S.; Elgarhy, Gehad S.; El-Subruiti, Gehan M.; Omer, Ahmed M.
      International Journal of Biological Macromolecules (2020), 154 (), 307-318CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      An efficient composite adsorbent was fabricated based on CM-cellulose (CMC) microbeads incorporated carboxylated graphene oxide (GOCOOH) for the adsorptive removal of cationic methylene blue dye (MB). The developed CMC/GOCOOH composite microbeads were characterized by means of FTIR, TGA, SEM, XPS, BET and zeta potential anal. tools. Various parameters affecting the removal of MB dye such as the amt. of GOCOOH, initial MB concn., adsorbent dosage, pH and medium temp. were optimized using a series of batch adsorption expts. The exptl. data of the adsorption process were more fitted to Langmuir isotherm (R2 = 0.998) with a max. adsorption capacity of 180.32 mg/g and followed the pseudo-second order kinetic model. Moreover, the adsorption of MB dye onto CMC/GOCOOH composite microbeads was an exothermic process with a max. capacity at pH 10. Besides, the fabricated adsorbent exposed also better reusability for nine repetitive cycles with highly adsorption properties. The gained results imply that the CMC/GOCOOH microbeads could be potentially applied as an effective and reusable adsorbent for MB dye removal from aq. solns.
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    55. 55
      Chan, C. H.; Chia, C. H.; Zakaria, S.; Sajab, M. S.; Chin, S. X. Cellulose nanofibrils: a rapid adsorbent for the removal of methylene blue. RSC Adv. 2015, 5, 18204– 18212,  DOI: 10.1039/c4ra15754k
      55
      Cellulose nanofibrils: a rapid adsorbent for the removal of methylene blue
      Chan, Chi Hoong; Chia, Chin Hua; Zakaria, Sarani; Sajab, Mohd. Shaiful; Chin, Siew Xian
      RSC Advances (2015), 5 (24), 18204-18212CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
      Cellulose nanofibrils (CNF) were prepd. from kenaf core (KC) using acidified-chlorite bleaching method and followed by disintegration using a high speed blender. The effects of disintegration time and acid treatment on the defibrillation of holocellulose were studied. Hemicellulose was found to facilitate defibrillation, as CNF without any acid treatment was fully defibrillated after 30 min. The adsorption kinetics of CNF toward cationic dye cannot be accurately detd. due to its quick adsorption performance, in which the equil. is achieved immediately after 1 min of contact time. The effects of acid treatment on holocellulose, pH, adsorbent dosage, temp. and dye concn. were studied and optimized. Adsorption data were fitted to both Langmuir and Freundlich models where the Langmuir model was found to be the better model to describe the adsorption process. The max. adsorption capacity was found to be 122.2 mg g-1 at pH 9, 20 °C for the non-acid treated CNF. The CNF can be regenerated by desorption at low pH where as much as 70% of the dye adsorbed can be desorbed after 6 cycles of adsorption-desorption.
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    56. 56
      Nguyen, V. T.; Ha, L. Q.; Nguyen, T. D. L.; Ly, P. H.; Nguyen, D. M.; Hoang, D. Nanocellulose and Graphene Oxide Aerogels for Adsorption and Removal Methylene Blue from an Aqueous Environment. ACS Omega 2022, 7, 1003– 1013,  DOI: 10.1021/acsomega.1c05586
      56
      Nanocellulose and graphene oxide aerogels for adsorption and removal methylene blue from aqueous environment
      Nguyen, Vy T.; Ha, Lam Q.; Nguyen, Tu D. L.; Ly, Phuong H.; Nguyen, Dang Mao; Hoang, DongQuy
      ACS Omega (2022), 7 (1), 1003-1013CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      The characteristics of aerogel materials such as the low d. and large surface area enable them to adsorb large amts. of substances, so they show great potential for application in industrial wastewater treatment. Herein, using a combination of completely environmentally friendly materials such as cellulose nanofibers (CNFs) extd. from the petioles of the nipa palm tree and graphene oxide (GO) fabricated by simple solvent evapn., a composite aerogel was prepd. by a freeze-drying method. The obtained aerogel possessed a light d. of 0.0264 g/cm3 and a porosity of more than 98.2%. It was able to withstand a wt. as much as 2500 times with the max. force (1479.5 N) to break up 0.2 g of an aerogel by compression strength testing and was stable in the aquatic environment, enabling it to be reused five times with an adsorption capacity over 90%. The CNF/GO aerogel can recover higher than 85% after 30 consecutive compression recovery cycles, which is convenient for the reusability of this material in wastewater treatments. The obtained aerogel also showed a good interaction between the component phases, a high thermal stability, a 3D network structure combined with thin walls and pores with a large sp. surface area. In addn., the aerogel also exhibited a fast adsorption rate for methylene blue (MB) adsorption, a type of waste from the textile industry that pollutes water sources, and it can adsorb more than 99% MB in water in less than 20 min. The excellent adsorption of MB onto the CNF/GO aerogel was driven by electrostatic interactions, which agreed with the pseudo-second-order kinetic model with a correlation coeff. R2 = 0.9978. The initial results show that the CNF/GO aerogel is a highly durable "green" light material that might be applied in the treatment of domestic org. waste water and is completely recoverable and reusable.
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    57. 57
      Huang, J.; Yan, Z. Adsorption Mechanism of Oil by Resilient Graphene Aerogels from Oil–Water Emulsion. Langmuir 2018, 34, 1890– 1898,  DOI: 10.1021/acs.langmuir.7b03866
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      Adsorption Mechanism of Oil by Resilient Graphene Aerogels from Oil-Water Emulsion
      Huang, Jiankun; Yan, Zifeng
      Langmuir (2018), 34 (5), 1890-1898CODEN: LANGD5; ISSN:0743-7463. (American Chemical Society)
      A facile synthesis strategy was adopted to prep. resilient graphene aerogel (GA) with properties of high emulsified oil adsorption capacities, excellent rebounding performance, oil-water selectivity, and recycling abilities. The max. adsorption capacity of GA for emulsified diesel oil was 2.5 × 104 mg g-1. The microscopic kinetic and thermodn. mutual reaction models of diesel oil emulsion adsorption onto GA were investigated to describe the adsorption mechanism. The emulsified diesel oil was able to be sepd. efficiently from the oil-water emulsion by GA because of their high oil selectivity. Interestingly, both kinetics and thermodn. expts. show that emulsified oil adsorption on GA is a phys. adsorption and spontaneous process. Besides, GA can be reused with prominent repeatability for at least 10 cycles, demonstrating feasibility in practical applications of GA-based oily water treatment.
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    58. 58
      Luo, M.; Wang, M.; Pang, H.; Zhang, R.; Huang, J.; Liang, K.; Chen, P.; Sun, P.; Kong, B. Super-assembled highly compressible and flexible cellulose aerogels for methylene blue removal from water. Chin. Chem. Lett. 2021, 32, 2091– 2096,  DOI: 10.1016/j.cclet.2021.03.024
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      Super-assembled highly compressible and flexible cellulose aerogels for methylene blue removal from water
      Luo, Mingfu; Wang, Meng; Pang, Huaipeng; Zhang, Runhao; Huang, Jing; Liang, Kang; Chen, Pu; Sun, Peipei; Kong, Biao
      Chinese Chemical Letters (2021), 32 (6), 2091-2096CODEN: CCLEE7; ISSN:1001-8417. (Elsevier B.V.)
      Phys. adsorption is a common method to solve the contamination of methylene blue in dyeing wastewater. As a kind of adsorption material, cellulose aerogels with high porosity and surface areas have great potential application in methylene blue removal. However, the week hydrogen bonding between cellulose nanofibers making the cellulose aerogels with the poor mech. properties and can be easily destroyed during adsorption. Hence, the prepn. of cellulose aerogels with high mech. strength is still a great challenge. Here, we report a robust super-assembly strategy to fabricate cellulose aerogels by combining cellulose nanofibers with PVA and M-K10. The resulting cellulose aerogels not only has a robust chem. cross-linked network, but also has strong H-bonds, which greatly enhance the mech. properties. The resulting cellulose aerogels possess a low d. of 19.32 mg/cm3. Furthermore, the cellulose aerogel shows 93% shape recovery under 60% strain (9.5 kPa under 60% strain) after 100 cycles, showing excellent mech. property. The adsorption capacity of cellulose aerogel to methylene blue soln. of 20 mg/L is 2.28 mg/g and the adsorption kinetics and adsorption isotherms have also been studied. Pseudo-second-order kinetic model and Freundlich isotherm model are more acceptable for indicating the adsorption process of methylene blue on the cellulose aerogel. Thus, this compressible and durable cellulose aerogel is a very prospective material for dyeing wastewater cleanup.
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    59. 59
      Phuong, N. T. X.; Ho, K. H.; Nguyen, C. T. X.; Dang, Y. T.; Do, N. H. N.; Le, K. A.; Do, T. C. Novel Fabrication of Renewable Aerogels from Coconut Coir Fibers for Dye Removal. Chem. Eng. Trans. 2021, 89, 31,  DOI: 10.3303/CET2189006
      There is no corresponding record for this reference.
    60. 60
      Hosseini, H.; Zirakjou, A.; McClements, D. J.; Goodarzi, V.; Chen, W.-H. Removal of methylene blue from wastewater using ternary nanocomposite aerogel systems: Carboxymethyl cellulose grafted by polyacrylic acid and decorated with graphene oxide. J. Hazard. Mater. 2022, 421, 126752,  DOI: 10.1016/j.jhazmat.2021.126752
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      Removal of methylene blue from wastewater using ternary nanocomposite aerogel systems: Carboxymethyl cellulose grafted by polyacrylic acid and decorated with graphene oxide
      Hosseini, Hadi; Zirakjou, Abbas; McClements, David Julian; Goodarzi, Vahabodin; Chen, Wei-Hsin
      Journal of Hazardous Materials (2022), 421 (), 126752CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
      In this study, environmentally-friendly nanocomposite hydrogels were fabricated. These hydrogels consisted of semi-interpenetrating networks of CM-cellulose (CMC) mols. grafted to polyacrylic acid (PAA), as an eco-friendly and non-toxic polymer with numerous carboxyl and hydroxyl functional groups, which were reinforced with different levels of graphene oxide particles (0.5, 1.5 or 3% wt). Field-emission electron scanning microscopy (FESEM) images indicated that the pore size of the nanocomposites decreased with increasing graphic oxide concn. The presence of the graphic oxide increased the storage modulus and thermal stability of the nanocomposite hydrogels. The hydrogels had an adsorption capacity of 138 mg/g of a model cationic dye pollutant (methylene blue) after 250 min. Moreover, a reusability test showed that the adsorption capacity remained at around 90% after 9 cycles. D. functional theory (DFT) simulations suggested that the adsorption of methylene blue was mainly a result of π-π bonds, hydrogen bonds, and electrostatic interactions with graphene oxide. Our results indicated that the nanocomposite hydrogels fabricated in this study may be eco-friendly, stable, efficient, and reusable adsorbents for ionic pollutants in wastewater treatment.
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    61. 61
      Ahmad, T.; Danish, M.; Rafatullah, M.; Ghazali, A.; Sulaiman, O.; Hashim, R.; Ibrahim, M. N. M. The use of date palm as a potential adsorbent for wastewater treatment: a review. Environ. Sci. Pollut. Res. 2012, 19, 1464– 1484,  DOI: 10.1007/s11356-011-0709-8
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      The use of date palm as a potential adsorbent for wastewater treatment: a review
      Ahmad, Tanweer; Danish, Mohammad; Rafatullah, Mohammad; Ghazali, Arniza; Sulaiman, Othman; Hashim, Rokiah; Ibrahim, Mohamad Nasir Mohamad
      Environmental Science and Pollution Research (2012), 19 (5), 1464-1484CODEN: ESPLEC; ISSN:0944-1344. (Springer)
      A review. Background In tropical countries, the palm tree is one of the most abundant and important trees. Date palm is a principal fruit grown in many regions of the world. It is abundant, locally available and effective material that could be used as an adsorbent for the removal of different pollutants from aq. soln. Review This article presents a review on the role of date palm as adsorbents in the removal of unwanted materials such as acid and basic dyes, heavy metals, and phenolic compds. Many studies on adsorption properties of various low cost adsorbent, such as agricultural waste and activated carbons based on agricultural waste have been reported in recent years. Conclusion Studies have shown that date palm-based adsorbents are the most promising adsorbents for removing unwanted materials. No previous review is available where researchers can get an overview of the adsorption capacities of date palm-based adsorbent used for the adsorption of different pollutants. This review provides the recent literature demonstrating the usefulness of date palm biomass-based adsorbents in the adsorption of various pollutants.
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    62. 62
      Nguyen, K. D.; Vo, N. T.; Le, K. T. M.; Ho, K. V.; Phan, N. T. S.; Ho, P. H.; Le, H. V. Defect-engineered metal–organic frameworks (MOF-808) towards the improved adsorptive removal of organic dyes and chromium (vi) species from water. New J. Chem. 2023, 47, 6433– 6447,  DOI: 10.1039/d2nj05693c
      62
      Defect-engineered metal-organic frameworks (MOF-808) towards the improved adsorptive removal of organic dyes and chromium(VI) species from water
      Nguyen, Khoa D.; Vo, Nhi T.; Le, Khanh T. M.; Ho, Khanh V.; Phan, Nam T. S.; Ho, Phuoc H.; Le, Ha V.
      New Journal of Chemistry (2023), 47 (13), 6433-6447CODEN: NJCHE5; ISSN:1144-0546. (Royal Society of Chemistry)
      Two defective Zr-based metal-org. frameworks (Zr-MOFs), MOF-808-OH and MOF-808-NH2, were synthesized by partially replacing the 1,3,5-benzenetricarboxylate building block with 5-hydroxyisophthalate and 5-aminoisophthalate, resp. The structural features of the defective materials were analyzed by powder x-ray diffraction (PXRD), SEM, N physisorption at 77 K, and TGA. Importantly, the no. of defect sites detd. via 1H NMR (1H-NMR) anal. of the digested materials was ∼7 mol% for MOF-808-OH and 3 mol% for MOF-808-NH2. The presence of the defect sites increased the no. of acidic centers on Zr-clusters originating from missing-linker nodes which accounted for a remarkable adsorption capacity towards various anionic org. dyes and Cr(VI) species. Compared to std. MOF-808, the defect-engineered ones showed significant increments by 30-60% in trapping capacity for anionic contaminants including sunset yellow, quinoline yellow, Methyl orange, and K dichromate, while they exhibited modest improvements by 5-15% in the removal of cationic dyes, malachite green and methylene blue.
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    63. 63
      Elsayed, I.; Schueneman, G. T.; El-Giar, E. M.; Hassan, E. B. Amino-Functionalized Cellulose Nanofiber/Lignosulfonate New Aerogel Adsorbent for the Removal of Dyes and Heavy Metals from Wastewater. Gels 2023, 9, 154,  DOI: 10.3390/gels9020154
      63
      Amino-Functionalized Cellulose Nanofiber/Lignosulfonate New Aerogel Adsorbent for the Removal of Dyes and Heavy Metals from Wastewater
      Elsayed, Islam; Schueneman, Gregory T.; El-Giar, Emad M.; Hassan, El Barbary
      Gels (2023), 9 (2), 154CODEN: GELSAZ; ISSN:2310-2861. (MDPI AG)
      Due to the increasingly widespread water pollutants and the high cost of treatment methods, there is a demand for new, inexpensive, renewable, and biodegradable adsorbent materials for the purifn. of wastewater contaminants. In this study, a new biocomposite aerogel (Amf-CNF/LS) was prepd. using a chem. crosslinking method between the amino-functionalized cellulose nanofibers (Amf-CNF) and lignosulfonates (LS). The phys. and chem. properties of the prepd. aerogel were investigated using several techniques including elemental anal., SEM (SEM-EDS), Fourier transform IR spectroscopy (FTIR), thermal gravimetric anal. (TGA), and N2 adsorption-desorption anal. The Amf-CNF/LS aerogel was then applied for the removal of methylene blue (MB), rhodamine B dye (RhB), and the heavy metal cadmium ion (Cd2+) from synthetic wastewater solns. The adsorption parameters controlling the adsorption process including the pH, contact time, adsorbent dosage, and adsorbate concen-tration were optimized. High adsorption kinetics and isotherms were obsd., with the adsorption isotherms of the Amf-CNF/LS aerogel fitting the Langmuir model with max. adsorption capacities of 170.94, 147.28, and 129.87 mg/g for MB, RhB, and Cd2+, resp. These results show that Amf-CNF/LS aerogel is a promising green and inexpensive adsorbent for MB, RhB, and Cd2+ removal from wastewater.
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    64. 64
      Salazar-Rabago, J. J.; Leyva-Ramos, R.; Rivera-Utrilla, J.; Ocampo-Perez, R.; Cerino-Cordova, F. J. Biosorption mechanism of Methylene Blue from aqueous solution onto White Pine (Pinus durangensis) sawdust: Effect of operating conditions. Sustainable Environ. Res. 2017, 27, 32– 40,  DOI: 10.1016/j.serj.2016.11.009
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      Biosorption mechanism of Methylene Blue from aqueous solution onto White Pine (Pinus durangensis) sawdust: Effect of operating conditions
      Salazar-Rabago, Jacob J.; Leyva-Ramos, Roberto; Rivera-Utrilla, Jose; Ocampo-Perez, Raul; Cerino-Cordova, Felipe J.
      Sustainable Environment Research (2017), 27 (1), 32-40CODEN: SERUBY; ISSN:2468-2039. (Elsevier B.V.)
      In this work, the biosorption mechanism of the cationic dye Methylene Blue (MB) on natural White Pine sawdust (NS) (Pinus durangensis) was investigated. Likewise, the surface charge distribution of NS was detd., and its point of zero charge was found to be 4.3. Besides, the capacity of the NS for adsorbing MB was increased 1.7, 2.0 and 4.6 times when the pH was raised from 3 to 4.25, 3 to 7 and 3 to 10, resp. This behavior was attributed to the electrostatic attraction between the neg. charged surface of NS and the cationic species MB+. The adsorption capacity increased with increased temp. because the adsorption was an endothermic process. The adsorption capacity was drastically reduced by increasing the ionic strength of the soln. corroborating with the fact that the electrostatic attractions played a crucial role in the adsorption of MB on NS. It was also shown that the MB was chemisorbed because the adsorption was not reversible. The predominant adsorption mechanisms were the electrostatic attraction and chemisorption and not ion exchange.
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    65. 65
      Bialik, E.; Stenqvist, B.; Fang, Y.; Östlund, Å.; Furó, I.; Lindman, B.; Lund, M.; Bernin, D. Ionization of Cellobiose in Aqueous Alkali and the Mechanism of Cellulose Dissolution. J. Phys. Chem. Lett. 2016, 7, 5044– 5048,  DOI: 10.1021/acs.jpclett.6b02346
      65
      Ionization of Cellobiose in Aqueous Alkali and the Mechanism of Cellulose Dissolution
      Bialik, Erik; Stenqvist, Bjoern; Fang, Yuan; Oestlund, Aasa; Furo, Istvan; Lindman, Bjoern; Lund, Mikael; Bernin, Diana
      Journal of Physical Chemistry Letters (2016), 7 (24), 5044-5048CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
      Cellulose, one of the most abundant renewable resources, is insol. in most common solvents but dissolves in aq. alkali under a narrow range of conditions. To elucidate the solubilization mechanism, we performed electrophoretic NMR on cellobiose, a subunit of cellulose, showing that cellobiose acts as an acid with two dissocn. steps at pH 12 and 13.5. Chem. shift differences between cellobiose in NaOH and NaCl were estd. using 2D NMR and compared to DFT shift differences upon deprotonation. The dissocn. steps are the deprotonation of the hemiacetal OH group and the deprotonation of one of four OH groups on the nonreducing anhydroglucose unit. MD simulations reveal that aggregation is suppressed upon charging cellulose chains in soln. Our findings strongly suggest that cellulose is to a large extent charged in concd. aq. alkali, a seemingly crucial factor for solubilization. This insight, overlooked in the current literature, is important for understanding cellulose dissoln. and for synthesis of new sustainable materials.
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    66. 66
      Swensson, B.; Larsson, A.; Hasani, M. Probing Interactions in Combined Hydroxide Base Solvents for Improving Dissolution of Cellulose. Polymers 2020, 12, 1310,  DOI: 10.3390/polym12061310
      66
      Probing interactions in combined hydroxide base solvents for improving dissolution of cellulose
      Swensson, Beatrice; Larsson, Anette; Hasani, Merima
      Polymers (Basel, Switzerland) (2020), 12 (6), 1310CODEN: POLYCK; ISSN:2073-4360. (MDPI AG)
      To further understand cellulose-solvent interactions in aq. hydroxide solns., cellulose behavior in aq. solns. of NaOH combined with tetramethylammonium hydroxide (TMAH) or benzyltrimethylammonium hydroxide (Triton B), as well as urea, was investigated. The rheol. properties of the solns. were assessed through flow sweeps at different temps., and the intermol. interactions were probed using solvatochromic dyes. The results showed that NaOH combined with TMAH had synergistic effects on cellulose dissoln. and was a better solvent for cellulose than the combination of NaOH with Triton B, in spite of the superior dissoln. ability of Triton B alone. This somewhat unexpected finding shows that the base pair needs to be selected with care. Interestingly, addn. of urea had no significant effect on the solvatochromic parameters or dissoln. capacity of solns. of Triton B but rendered improved stability of solns. contg. NaOH and/or TMAH. It seems that both urea and Triton B weaken the hydrophobic assembly effect of these solns., but urea is excluded from interacting with cellulose in the presence of Triton B. This study provides further insight into dissoln. of cellulose and the possibility of utilizing combinations of hydroxide bases to achieve improved soln. properties.
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    67. 67
      Wei, X.; Huang, T.; Nie, J.; Yang, J.-h.; Qi, X.-d.; Zhou, Z.-w.; Wang, Y. Bio-inspired functionalization of microcrystalline cellulose aerogel with high adsorption performance toward dyes. Carbohydr. Polym. 2018, 198, 546– 555,  DOI: 10.1016/j.carbpol.2018.06.112
      67
      Bio-inspired functionalization of microcrystalline cellulose aerogel with high adsorption performance toward dyes
      Wei, Xiao; Huang, Ting; Nie, Jun; Yang, Jing-hui; Qi, Xiao-dong; Zhou, Zuo-wan; Wang, Yong
      Carbohydrate Polymers (2018), 198 (), 546-555CODEN: CAPOD8; ISSN:0144-8617. (Elsevier Ltd.)
      As one of the materials from natural resources, the functionalization and application of cellulose attract increasing concerns. In this work, we reported a facile method to prep. the bio-inspired functionalization of microcryst. cellulose (MCC) aerogel through polydopamine (PDA) coating, which was realized via the self-polymn. of dopamine in the MCC/LiBr soln. followed by the freeze-drying technol. The morphol. characterization showed that the pore morphologies of the compounded aerogel were influenced by the content of PDA. Adsorption measurements toward methylene blue (MB) showed that the compounded aerogel had high adsorption ability. Moreover, the compounded MCC/PDA aerogel exhibited excellent adsorption selectivity and it exhibited high efficiency to remove MB from different solns., such as the mixed soln. with anionic dyestuffs, the mixed soln. with cationic dyestuffs and the mixed soln. with common salt (NaCl). The high adsorption ability and excellent adsorption selectivity endows the compounded MCC/PDA aerogel with great potential applications in wastewater treatment.
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    68. 68
      Wan, C.; Zhang, L.; Yong, K.-T.; Li, J.; Wu, Y. Recent progress in flexible nanocellulosic structures for wearable piezoresistive strain sensors. J. Mater. Chem. C 2021, 9, 11001– 11029,  DOI: 10.1039/d1tc02360h
      68
      Recent progress in flexible nanocellulosic structures for wearable piezoresistive strain sensors
      Wan, Caichao; Zhang, Luyu; Yong, Ken-Tye; Li, Jian; Wu, Yiqiang
      Journal of Materials Chemistry C: Materials for Optical and Electronic Devices (2021), 9 (34), 11001-11029CODEN: JMCCCX; ISSN:2050-7534. (Royal Society of Chemistry)
      A review. With the coming of the "green" and "wearable" era, the superior flexibility and high biocompatibility accompanied by superb sensing abilities of nanocellulosic materials have significantly promoted the application of piezoresistive strain sensors in the area of intelligent wearable and skin-attachable devices (such as human motion detectors, human-machine interfaces, and electronic skins). In this review, a detailed overview on the design and prepn. strategies of nanocellulosic piezoresistive strain sensors is presented. The roles of nanocellulose in the core design parameters including sensitivity (gauge factor), dynamic durability, stretchability, hysteresis, and biocompatibility are summarized based on three primary points, namely the structure-response relationship, supramol. interaction, and synergistic mechanism. Furthermore, a comprehensive overview of the fundamental aspects related to the origin, physicochem. properties, and disassembly-reassembly approaches of nanocellulose is provided, and an anal. on the morphol. and mech. properties of 1D-to-3D nanocellulose assemblies is also illustrated. Finally, this review presents a brief summary, challenges, and perspectives of nanocellulosic strain sensors.
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    69. 69
      Wang, S.; Zhang, Q.; Wang, Z.; Pu, J. Facile fabrication of an effective nanocellulose-based aerogel and removal of methylene blue from aqueous system. J. Water Process Eng. 2020, 37, 101511,  DOI: 10.1016/j.jwpe.2020.101511
      There is no corresponding record for this reference.
    70. 70
      Nguyen, H. H. M.; Tan, K. V. M.; Van, T. T. T.; Nguyen, H. N.; Phan, A. N. Q.; Tran, A. T. T.; Le, P. K.; Le, K. A.; Nguyen, K. D.; Le, H. V. Preparation of Cu-modified bacterial cellulose aerogels derived from nata de coco towards the enhanced adsorption of hydrophobic organic solvents. J. Porous Mater. 2023, 30, 1195– 1205,  DOI: 10.1007/s10934-022-01413-z
      70
      Preparation of Cu-modified bacterial cellulose aerogels derived from nata de coco towards the enhanced adsorption of hydrophobic organic solvents
      Nguyen, Hanh H. M.; Tan, Khang V. M.; Van, Thanh T. T.; Nguyen, Hanh N.; Phan, Anh N. Q.; Tran, An T. T.; Le, Phung K.; Le, Kien A.; Nguyen, Khoa D.; Le, Ha V.
      Journal of Porous Materials (2023), 30 (4), 1195-1205CODEN: JPMAFX; ISSN:1380-2224. (Springer)
      This study presented a simple and eco-friendly method to load copper nanoparticles on the surface of bacterial cellulose from nata de coco produced via the fermn. of coconut water by Acetobacter xylinum. The Cu modification of BC surface was based on the redn. of copper (II) acetate by hydrazine under ambient conditions in a dispersion system of Nata de coco in water, which was followed by freeze-drying, affording lightwt. Cu-contg. cellulose aerogels. The structural features of the obtained aerogels were investigated by SEM with energy dispersive X-ray anal. (SEM/EDX), thermogravimetric anal. (TGA), powder X-ray diffraction (PXRD), and nitrogen physisorption, indicating the high cellulose crystallinity, three-dimensional matrix and homogenous dispersion of Cu species on the cellulose bundles. The Cu-modified aerogel exhibited a significantly improved adsorption capacity of cyclohexane (66.4 g/g) as compared to that of pure cellulose (45 g/g). The excellent performances of 65.1-109.6 g/g were also obsd. for other water-insol. liqs. including n-hexane, toluene, THF, Et acetate, chlorobenzene, 1,2-dichlorobenzene, dichloromethane, and chloroform depending their d.
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    71. 71
      Nath, P. C.; Ojha, A.; Debnath, S.; Neetu, K.; Bardhan, S.; Mitra, P.; Sharma, M.; Sridhar, K.; Nayak, P. K. Recent advances in valorization of pineapple (Ananas comosus) processing waste and by-products: A step towards circular bioeconomy. Trends Food Sci. Technol. 2023, 136, 100– 111,  DOI: 10.1016/j.tifs.2023.04.008
      71
      Recent advances in valorization of pineapple (Ananas comosus) processing waste and by-products: A step towards circular bioeconomy
      Nath, Pinku Chandra; Ojha, Amiya; Debnath, Shubhankar; Neetu, Kumari; Bardhan, Sayan; Mitra, Priya; Sharma, Minaxi; Sridhar, Kandi; Nayak, Prakash Kumar
      Trends in Food Science & Technology (2023), 136 (), 100-111CODEN: TFTEEH; ISSN:0924-2244. (Elsevier Ltd.)
      One of the most significant and challenging tasks on the planet is using fruit and vegetable wastes in the food processing industries. This waste disposal requires a substantial capital investment, the majority of which is for transportation. As a result, these wastes are dumped and burned in open areas. Thus, valorization strategies must be implemented in order to minimize the fruit and vegetables waste. This article reviewed the characteristics and nutritional compn. of pineapple wastes (PAWs), different waste parts of pineapple and their economic significance, utilization of high-value added products, and the benefits of employing PAWs in a variety of food applications. Pineapple has become a delicious fruit in recent times due to its unique aroma, an abundance of volatile chems., and nutritional content. The tropical fruit's pulp, skin, and leaves may provide a source of natural anti-microbial and antioxidant chems. From a socioeconomic point of view, PAW has the potential to become a new source of raw materials for the industries and could potentially replace the existing sources, which are both expensive and non-renewable. The bromelain enzyme extd. from pineapple and other key value-added products could be utilized in the food manufg. industry, thereby contributing to healthy food and a sustainable environment. Although studies have been conducted on a small scale, more investigation into the techno-economic viability of the biorefinery's processes is needed to ensure a smooth transition to a sustainable economy with minimal impact on the environment.
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    72. 72
      Meneses, I. P.; Novaes, S. D.; Dezotti, R. S.; Oliveira, P. V.; Petri, D. F. S. CTAB-modified carboxymethyl cellulose/bagasse cryogels for the efficient removal of bisphenol A, methylene blue and Cr(VI) ions: Batch and column adsorption studies. J. Hazard. Mater. 2022, 421, 126804,  DOI: 10.1016/j.jhazmat.2021.126804
      72
      CTAB-modified carboxymethyl cellulose/bagasse cryogels for the efficient removal of bisphenol A, methylene blue and Cr(VI) ions: Batch and column adsorption studies
      Meneses, Izabo Pereira; Novaes, Stephanie Dias; Dezotti, Rafael Sobral; Oliveira, Pedro Vitoriano; Petri, Denise Freitas Siqueira
      Journal of Hazardous Materials (2022), 421 (), 126804CODEN: JHMAD9; ISSN:0304-3894. (Elsevier B.V.)
      The simultaneous removal of org. and inorg. pollutants from water requires multifunctional adsorbents. Cryogels of CM-cellulose (CMC) and sugarcane bagasse (BG) were modified with cetyltrimethylammonium bromide (CTAB) micelles for the adsorption of methylene blue (MB), Cr(VI) ions and bisphenol A (BPA) sep., in binary or ternary aq. mixts. Batch adsorption studies of MB and Cr(VI) and BPA on the CMCBG-CTAB adsorbents indicated removal capacities of 100%, 70% and 95%, resp. MB adsorbed as multilayers on the CMCBG walls by electrostatic interaction, whereas Cr(VI) and BPA adsorbed on the cationic CTAB micelles surface and hydrophobic core of CTAB micelles, resp. The breakthrough curves obtained for pure adsorbates and their mixts. showed that the adsorption of Cr(VI) ions increased (i) ∼ 3.5 times in binary mixt. with BPA or in the ternary mixt., in comparison to pure Cr(VI) soln., and (ii) 1.4 times in binary mixt. with MB mols., due to synergistic effects. In the presence of Cr(VI) ions in binary or ternary mixts., the adsorption of MB was dramatically reduced due to screening effects. The adsorption of BPA was not significantly affected by the presence of MB or Cr(VI). The adsorbents were recycled five times without significant efficiency loss.
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    73. 73
      Liu, X.; Zhou, Y.; Nie, W.; Song, L.; Chen, P. Fabrication of hydrogel of hydroxypropyl cellulose (HPC) composited with graphene oxide and its application for methylene blue removal. J. Mater. Sci. 2015, 50, 6113– 6123,  DOI: 10.1007/s10853-015-9166-y
      73
      Fabrication of hydrogel of hydroxypropyl cellulose (HPC) composited with graphene oxide and its application for methylene blue removal
      Liu, Xiaoyan; Zhou, Yifeng; Nie, Wangyan; Song, Linyong; Chen, Pengpeng
      Journal of Materials Science (2015), 50 (18), 6113-6123CODEN: JMTSAS; ISSN:0022-2461. (Springer)
      Novel environmental friendly hydroxypropyl cellulose (HPC) hydrogels were fabricated upon compositing with graphene oxide (GO) in this work. In order to promote a more homogeneous dispersion of GO sheets in HPC, GO was firstly modified with HPC chains through esterification. The morphol. and chem. structure of the functionalized HPC-GO were characterized by transmission electron microscopy, XPS, Fourier transform IR spectrometer, X-ray diffraction, and thermo-gravimetric anal. Then scanning electronic microscope was employed to compare the morphologies of the HPC and HPC-GO/HPC hydrogels. The obtained HPC-GO/HPC hydrogels exhibited excellent adsorption performance toward methylene blue. Simulation of the practical use by prepg. simple adsorption columns made from in situ formation of HPC-based hydrogels had given a visible observation of the significant adsorption effect brought by the incorporation of HPC-GO sheets. Adsorption kinetics were then imitated by Lagergren pseudo-first-order and pseudo-second-order models. Adsorption isotherms were imitated by Langmuir isotherm and Freundlich isotherm.
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    74. 74
      Hua, J.; Meng, R.; Wang, T.; Gao, H.; Luo, Z.; Jin, Y.; Liu, L.; Yao, J. Highly Porous Cellulose Microbeads and their Adsorption for Methylene Blue. Fibers Polym. 2019, 20, 794– 803,  DOI: 10.1007/s12221-019-8334-0
      74
      Highly Porous Cellulose Microbeads and their Adsorption for Methylene Blue
      Hua, Jiarui; Meng, Ranju; Wang, Tiejun; Gao, Huiying; Luo, Zhenze; Jin, Yuanyuan; Liu, Lin; Yao, Juming
      Fibers and Polymers (2019), 20 (4), 794-803CODEN: FPIOA6; ISSN:1229-9197. (Korean Fiber Society)
      Highly porous cellulose microbeads with porosity of more than 90% were successfully prepd. via a facile dissoln. and subsequent regeneration of cellulose in H2SO4/Na2SO4 coagulation bath. Effects of coagulation temp., H2SO4, and Na2SO4 concn. on the microstructure, av. diam., porosity, sp. surface area, and mech. property of formed cellulose beads were investigated systematically. In view of the high porosity and specific area, the cellulose beads were used as adsorbents for dye removal. The results revealed that the porous cellulose beads exhibited high adsorption performance with max. adsorption capacity of 48.80 mg/g for cationic dye methylene blue. Besides, the porous cellulose beads also presented a potential in practical application and its adsorption capacity for methylene blue still retained 29.43 mg/g after six adsorption-desorption cycles.
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    75. 75
      Batzias, F.; Sidiras, D.; Schroeder, E.; Weber, C. Simulation of dye adsorption on hydrolyzed wheat straw in batch and fixed-bed systems. Chem. Eng. J. 2009, 148, 459– 472,  DOI: 10.1016/j.cej.2008.09.025
      75
      Simulation of dye adsorption on hydrolyzed wheat straw in batch and fixed-bed systems
      Batzias, Fragiskos; Sidiras, Dimitris; Schroeder, Elisabeth; Weber, Christina
      Chemical Engineering Journal (Amsterdam, Netherlands) (2009), 148 (2-3), 459-472CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
      The simulation of batch and column kinetics of Methylene Blue and Red Basic 22 adsorption on mild acid hydrolyzed wheat straw was investigated, using untreated wheat straw as control, in order to examine its properties for potential use as a low cost adsorbent for wastewater dye removal. The BET surface area, the adsorption capacities (estd. according to Freundlich and Langmuir models), indicated that mild acid hydrolysis enhances significantly the adsorption properties of the original material. This enhancement can be attributed to the removal of the hemicelluloses during sulfuric acid treatment, resulting in the opening' of the pores of lignocellulosic matrix's structure and the increasing of the BET surface area.
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    76. 76
      Mahmoud, M. E.; Abdelwahab, M. S. Fabricated and functionalized magnetite/phenylenediamine/cellulose acetate nanocomposite for adsorptive removal of methylene blue. Int. J. Biol. Macromol. 2019, 128, 196– 203,  DOI: 10.1016/j.ijbiomac.2019.01.102
      76
      Fabricated and functionalized magnetite/phenylenediamine/cellulose acetate nanocomposite for adsorptive removal of methylene blue
      Mahmoud, Mohamed E.; Abdelwahab, Mohamed S.
      International Journal of Biological Macromolecules (2019), 128 (), 196-203CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      The industrial revolution in textile and dying process is moving with huge steps, but the treatment of produced wastewater from this industry is a huge dilemma. This work demonstrates the prepn. and utilization of cellulose acetate (CA) blended with Fe3O4 already chem. modified with O-phenylenediamine (PDA) to prep. a novel magnetic Fe3O4/PDA/CA nanocomposite. This nanomaterial was aimed to use in the removal of methylene blue (MB) dye from water. The adsorption process was conducted using a batch technique and the removal process was evaluated under various exptl. conditions. From this study, it was found that the values were increased from 55.8% to 88.54%, 45.5% to 84.8% and 42.56% to 76.45% by the increase of from pH 1 to 7, resp. using 10, 50 and 100 mg·L-1. The pseudo-second-order was found to be the most fitted model to confirm that the adsorption reaction is related to a chemisorption process between the Fe3O4/PDA/CA nanocomposite and MB dye. The Langmuir and Freundlich models were also found to best-fitted models to reveal the formation of monolayer and multilayer of MB over Fe3O4/PDA/CA nanocomposite in a chem. process. The thermodn. parameters confirm that this type of reaction is spontaneous and exothermic reaction.
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    77. 77
      Shi, H.; Li, W.; Zhong, L.; Xu, C. Methylene Blue Adsorption from Aqueous Solution by Magnetic Cellulose/Graphene Oxide Composite: Equilibrium, Kinetics, and Thermodynamics. Ind. Eng. Chem. Res. 2014, 53, 1108– 1118,  DOI: 10.1021/ie4027154
      77
      Methylene Blue Adsorption from Aqueous Solution by Magnetic Cellulose/Graphene Oxide Composite: Equilibrium, Kinetics, and Thermodynamics
      Shi, Haochun; Li, Weisong; Zhong, Lei; Xu, Chunjian
      Industrial & Engineering Chemistry Research (2014), 53 (3), 1108-1118CODEN: IECRED; ISSN:0888-5885. (American Chemical Society)
      In the present study, magnetic cellulose/graphene oxide composite (MCGO) was prepd. as a novel adsorbent to dispose of dye wastewater. The morphol. and chem. structure of the MCGO composite were characterized by the Fourier transform IR spectrometer (FT-IR), X-ray diffraction (XRD), and scanning electronic microscope (SEM). The adsorption of methylene blue (MB) onto MCGO was studied in relation to initial concn. of MB, contact time, adsorbent dose, and pH value of soln. Adsorption kinetics and the equil. adsorption isotherm were fitted by a pseudo-second-order kinetic model and Langmuir isotherm, resp. The thermodn. parameters indicated that the adsorption was spontaneous, favorable, and exothermic in nature. Furthermore, MCGO was very stable and can easily be recycled. The adsorption efficiency of MCGO was still over 89% after recycling for five times.
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    78. 78
      Oyewo, O. A.; Adeniyi, A.; Sithole, B. B.; Onyango, M. S. Sawdust-Based Cellulose Nanocrystals Incorporated with ZnO Nanoparticles as Efficient Adsorption Media in the Removal of Methylene Blue Dye. ACS Omega 2020, 5, 18798– 18807,  DOI: 10.1021/acsomega.0c01924
      78
      Sawdust-based cellulose nanocrystals incorporated with ZnO nanoparticles as efficient adsorption media in the removal of methylene blue dye
      Oyewo, Opeyemi A.; Adeniyi, Amos; Sithole, B. Bruce; Onyango, Maurice S.
      ACS Omega (2020), 5 (30), 18798-18807CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      The continuous increase in the wastes generated from forestry, timber, and paper industries has engendered the need for their transformation into economically viable materials for the benefit of mankind. This study reports the prepn. and application of sawdust-derived cellulose nanocrystals (CNC) incorporated with zinc oxide as a novel adsorbent for the removal of methylene blue (MB) from water. The CNC/ZnO nanocomposite was characterized using Fourier transform IR, X-ray diffraction (XRD), and SEM. The amt. of MB adsorbed was detd. by a UV-vis spectrophotometer. The microscopic anal. revealed that the nanocomposite had a narrow particle size range and exhibited both spherical and rod-like morphologies. The XRD anal. of the nanocomposite showed characteristic high-intensity peaks in the range of 30-75° attributed to the presence of ZnO nanoparticles, which were responsible for the enhancement of the crystallinity of the nanocomposite. The results revealed a relationship between the MB removal efficiency and changes in soln. pH, nanocomposite dosage, initial concn., temp., and reaction time. The adsorption equil. isotherm, measured in the temp. range of 25-45 °C and using a concn. of 20-100 mg/L, showed that the MB sorption followed the Langmuir isotherm with a max. adsorption capacity of 64.93 mg/g. A pseudo-second-order kinetic model gave the best fit to the exptl. data. Based on adsorption performance, the CNC/ZnO nanocomposite offers prospects for further research and application in amelioration of dye-contg. effluent.
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    79. 79
      Safavi-Mirmahalleh, S.-A.; Salami-Kalajahi, M.; Roghani-Mamaqani, H. Effect of surface chemistry and content of nanocrystalline cellulose on removal of methylene blue from wastewater by poly(acrylic acid)/nanocrystalline cellulose nanocomposite hydrogels. Cellulose 2019, 26, 5603– 5619,  DOI: 10.1007/s10570-019-02490-1
      79
      Effect of surface chemistry and content of nanocrystalline cellulose on removal of methylene blue from wastewater by poly(acrylic acid)/nanocrystalline cellulose nanocomposite hydrogels
      Safavi-Mirmahalleh, Seyedeh-Arefeh; Salami-Kalajahi, Mehdi; Roghani-Mamaqani, Hossein
      Cellulose (Dordrecht, Netherlands) (2019), 26 (9), 5603-5619CODEN: CELLE8; ISSN:0969-0239. (Springer)
      Nanocryst. cellulose (NCC) was modified with (3-aminopropyl)triethoxysilane (APTES) and hexadecyltrimethoxysilane (HDTMS) to obtain NCC-APTES and NCC-HDTMS resp. The modification was confirmed by Fourier transform IR (FT-IR) spectroscopy, X-ray diffraction (XRD) spectroscopy, thermogravimetric analyses (TGA), dynamic light scattering and zeta potential analyses. A series of poly(acrylic acid) (PAA)/NCC, PAA/NCC-APTES, and PAA/NCC-HDTMS hydrogel nanocomposites with various amts. of nanoparticles were synthesized by in situ radical polymn. method. Nanocomposites were characterized using XRD, TGA and field emission SEM. Also, swelling behavior of hydrogel nanocomposites showed that NCC and NCC-APTES helped swelling of hydrogels whereas CNN-HDTMS decreased swelling ratio. The hydrogel nanocomposites were also used as adsorbents for removal of methylene Blue from aq. soln. at different pH values. Results showed that the adsorption capacity for dye increased with increasing pH and contact time. Introducing NCC into hydrogel nanocomposite network affected adsorption capacity. Finally, adsorption kinetics was studied by three kinetic models including pseudo-first-order, pseudo-second-order and intra-particle diffusion models.
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    80. 80
      Cheng, J.; Zhan, C.; Wu, J.; Cui, Z.; Si, J.; Wang, Q.; Peng, X.; Turng, L.-S. Highly Efficient Removal of Methylene Blue Dye from an Aqueous Solution Using Cellulose Acetate Nanofibrous Membranes Modified by Polydopamine. ACS Omega 2020, 5, 5389– 5400,  DOI: 10.1021/acsomega.9b04425
      80
      Highly Efficient Removal of Methylene Blue Dye from an Aqueous Solution Using Cellulose Acetate Nanofibrous Membranes Modified by Polydopamine
      Cheng, Jiaqi; Zhan, Conghua; Wu, Jiahui; Cui, Zhixiang; Si, Junhui; Wang, Qianting; Peng, Xiangfang; Turng, Lih-Sheng
      ACS Omega (2020), 5 (10), 5389-5400CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      A new type of deacetylated cellulose acetate (DA)@polydopamine (PDA) composite nanofiber membrane was fabricated by electrospinning and surface modification. The membrane was applied as a highly efficient adsorbent for removing methylene blue (MB) from an aq. soln. The morphol., surface chem., surface wettability, and effects of operating conditions on MB adsorption ability, as well as the equil., kinetics, thermodn., and mechanism of adsorption, were systematically studied. The results demonstrated that a uniform PDA coating layer was successfully developed on the surface of DA nanofibers. The adsorption capacity of the DA@PDA nanofiber membrane reached up to 88.2 mg/g at a temp. of 25°C and a pH of 6.5 after adsorption for 30 h, which is about 8.6 times higher than that of DA nanofibers. The exptl. results showed that the adsorption behavior of DA@PDA composite nanofibers followed the Weber's intraparticle diffusion model, pseudo-second-order model, and Langmuir isothermal model. A thermodn. anal. indicated that endothermic, spontaneous, and physisorption processes occurred. Based on the exptl. results, the adsorption mechanism of DA@PDA composite nanofibers was also demonstrated.
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    81. 81
      Fang, Y.; Liu, Q.; Zhu, S. Selective biosorption mechanism of methylene blue by a novel and reusable sugar beet pulp cellulose/sodium alginate/iron hydroxide composite hydrogel. Int. J. Biol. Macromol. 2021, 188, 993– 1002,  DOI: 10.1016/j.ijbiomac.2021.07.192
      81
      Selective biosorption mechanism of methylene blue by a novel and reusable sugar beet pulp cellulose/sodium alginate/iron hydroxide composite hydrogel
      Fang, Yi; Liu, Qiang; Zhu, Siming
      International Journal of Biological Macromolecules (2021), 188 (), 993-1002CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      A cellulose-based sodium alginate/iron hydroxide (C/SA/Fe) composite hydrogel was fabricated by using epichlorohydrin as crosslinking agent as an effective adsorbent for dye. The physicochem. structure of the C/SA/Fe hydrogel was characterized by SEM, FTIR, XRD and TG. The adsorption performance for the removal of methylene blue (MB) was investigated. In addn., the selective adsorption of cationic dye was also studied. The FTIR anal. revealed that the Fe(OH)3 colloidal particles were successfully combined in the cellulose/sodium alginate hydrogel. The modified hydrogel had better adsorption performance, and the max. adsorption capacity of C/SA/Fe0.5 for MB was 105.93 mg/g according to the fitting results of adsorption isotherm. The kinetic study showed that the adsorption of MB onto C/SA/Fe was more consistent with the pseudo-second-order model, and was dominated by chemisorption mechanism such as ion exchange or electron sharing. The adsorption data fits well with the Langmuir model. Thermodn. anal. showed that the MB adsorption by C/SA/Fe was exothermic, spontaneous, favorable and feasible. After five adsorption-desorption cycles, the adsorption capacity was almost unchanged. So, the C/SA/Fe hydrogel is a potential material in the field of the recovery of agricultural byproducts or other bio-based cellulose, or environmental protection, etc.
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    82. 82
      Cao, X.; Liu, M.; Bi, W.; Lin, J.; Chen, D. D. Y. Direct carboxylation of cellulose in deep eutectic solvent and its adsorption behavior of methylene blue. Carbohydr. Polym. Technol. Appl. 2022, 4, 100222,  DOI: 10.1016/j.carpta.2022.100222
      82
      Direct carboxylation of cellulose in deep eutectic solvent and its adsorption behavior of methylene blue
      Cao, Xiwang; Liu, Min; Bi, Wentao; Lin, Jun; Chen, David Da Yong
      Carbohydrate Polymer Technologies and Applications (2022), 4 (), 100222CODEN: CPTACM; ISSN:2666-8939. (Elsevier Ltd.)
      The surface of cellulose particles was carboxylated (2.44 mmol/g) in a deep eutectic solvent contg. carboxylic acid. Based on the carboxyl content, the effects of key factors on cellulose carboxylation was systematically investigated. In addn., the reaction mechanism was studied by using liq. chromatog.-mass spectrometry, and the influence of deep eutectic solvent contg. carboxylic acid on the structure and physicochem. properties of cellulose during carboxylation was examd. using different characterization techniques. The results showed that the type of carboxylic acid, cellulose particle size, and pretreatment methods significantly affect the carboxylation efficiency, degrdn., and carbonization of cellulose. The internal crystal structure of cellulose did not change after the carboxylation reaction, while the surface crystal structure was destroyed by carboxylation, which greatly improved the dispersion and hydrophilicity properties of the product. The kinetics and thermodn. of carboxyl cellulose adsorption were studied as well. Potential application of carboxyl cellulose in the adsorption of pollutants was demonstrated. This study provides a new method for the direct modification of cellulose in deep eutectic solvents, as well as a new sustainable strategy for modifying other materials.
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    83. 83
      Beh, J. H.; Lim, T. H.; Lew, J. H.; Lai, J. C. Cellulose nanofibril-based aerogel derived from sago pith waste and its application on methylene blue removal. Int. J. Biol. Macromol. 2020, 160, 836– 845,  DOI: 10.1016/j.ijbiomac.2020.05.227
      83
      Cellulose nanofibril-based aerogel derived from sago pith waste and its application on methylene blue removal
      Beh, Jeng Hua; Lim, Teck Hock; Lew, Jin Hau; Lai, Jau Choy
      International Journal of Biological Macromolecules (2020), 160 (), 836-845CODEN: IJBMDR; ISSN:0141-8130. (Elsevier B.V.)
      Sago pith cellulose nanofibril (SPCNF) aerogel derived from sago pith waste (SPW) was successfully produced through three consecutive steps, namely dewaxing and delignification, ultra-sonication and homogenization and freeze drying. The aerogel was characterized using field emission SEM (FE-SEM), Fourier-transform infra-red spectroscopy (FTIR), X-ray diffraction (XRD) and thermogravimetric anal. (TGA). Results of the analyses collectively showed that lignin & hemicellulose were absent in the SPCNF aerogel product which has a high crystallinity index of 88%. The diams. of individual nanofibril constituents of the SPCNF were between 15 and 30 nm and aspect ratios >1000 were obsd. The SPCNF aerogel, with a d. measured at 2.1 mg/cm3, was efficient in methylene blue (MB) removal with a max. MB adsorption of 222.2 mg/g at 20°C. The adsorption of MB onto the SPCNF aerogel was rapid and found to follow a pseudo-second-order kinetic model with the adsorption isotherm being in congruence with the Langmuir model. The SPCNF aerogel exhibited outstanding MB removal efficacies with 5 mg and 20 mg of SPCNF capable of removing over 90% and almost 99% MB, resp. The optimized pH value and temp. for MB adsorption were detd. as pH 7 and 20°C.
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    84. 84
      Chong, K. Y.; Chia, C. H.; Zakaria, S.; Sajab, M. S.; Chook, S. W.; Khiew, P. S. CaCO3-decorated cellulose aerogel for removal of Congo Red from aqueous solution. Cellulose 2015, 22, 2683– 2691,  DOI: 10.1007/s10570-015-0675-2
      84
      CaCO3-decorated cellulose aerogel for removal of Congo Red from aqueous solution
      Chong, Kai Yin; Chia, Chin Hua; Zakaria, Sarani; Sajab, Mohd. Shaiful; Chook, Soon Wei; Khiew, Poi Sim
      Cellulose (Dordrecht, Netherlands) (2015), 22 (4), 2683-2691CODEN: CELLE8; ISSN:0969-0239. (Springer)
      The present study describes the prepn. of CaCO3-loaded cellulose aerogel and evaluation of its adsorptive removal of Congo Red (CR) from aq. soln. The CaCO3-cellulose aerogel was produced via in situ pptn. of CaCO3 into as-prepd. cellulose aerogel, which was prepd. by freeze-drying a crosslinked cellulose soln. that was dissolved using a NaOH/urea soln. The particles that formed in the aerogel were confirmed to be calcite CaCO3. Adsorption studies illustrated that the CR uptake by the aerogel was dependent on the dye concn. and temp. Incorporation of CaCO3 into the cellulose aerogel significantly enhanced the adsorption capacity of the aerogel toward CR. The max. adsorption capacity of the CaCO3-cellulose aerogel was approx. 75.81 mg/g.
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    85. 85
      Abramian, L.; El-Rassy, H. Adsorption kinetics and thermodynamics of azo-dye Orange II onto highly porous titania aerogel. Chem. Eng. J. 2009, 150, 403– 410,  DOI: 10.1016/j.cej.2009.01.019
      85
      Adsorption kinetics and thermodynamics of azo-dye Orange II onto highly porous titania aerogel
      Abramian, Lara; El-Rassy, Houssam
      Chemical Engineering Journal (Amsterdam, Netherlands) (2009), 150 (2-3), 403-410CODEN: CMEJAJ; ISSN:1385-8947. (Elsevier B.V.)
      We report herein a kinetic and thermodn. study of the adsorption of azo-dye Orange II from aq. solns. onto titania aerogels. Aerogels structure was confirmed by FTIR and N2 adsorption revealed their sp. surface area (500 m2/g), pore vol. (2.86 cm3/g) and pore size (mean 13.9 nm). Adsorption tests were conducted in batch reactors under various conditions where the effect of pH, temp., contact time, dye concn., and adsorbent dose were studied. Expts. performed at pH 2 show the optimal adsorption due to the best surface charge interactions. The temp. shows a weak influence with a decrease in the adsorption uptake as the temp. increases. Adsorption kinetics is shown to be very fast and follows a pseudo second-order indicating the coexistence of chemisorption and physisorption with the intra-particle diffusion being the rate controlling step. The exptl. data fit perfectly with Sips isotherms and reveal the ability of titania aerogel to adsorb 420 mg of Orange II per g of adsorbent at the optimal conditions. The thermodn. study reveals the activation energy (42.1 kJ/mol-1) and the changes in Gibbs free energy (1.2 kJ/mol-1), enthalpy (-16.4 kJ/mol-1), and entropy (-58 J/mol-1/K-1). The entire regeneration of the titania aerogel adsorption sites at pH 11 and 30° shows a total recovery of the dye and the efficient reusability and the economic interest of these adsorbing materials for environmental purposes.
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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.3c03130.

    • FTIR spectrum of fresh cellulose-based aerogel; determination of the zero-charge point (pHPZC) of the cellulose-based aerogel; UV–vis absorption spectra of the mixture of quinoline yellow and methylene blue (200 ppm:200 ppm) in the presence of cellulose-based aerogel at 30 °C and pH = 6.5; photographs of the collected samples after washing three times different solvents such as water, ethanol, acetone, and acetone solution containing 5 wt % of HCl; photographs of the regenerated aerogel after freeze-drying; and characterization of the used cellulose-based aerogel after the adsorption (PDF)


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