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Enhancement of Columbic Efficiency and Capacity of Li-Ion Batteries using a Boron Nitride Nanotubes-Dispersed-Electrolyte with High Ionic Conductivity
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Enhancement of Columbic Efficiency and Capacity of Li-Ion Batteries using a Boron Nitride Nanotubes-Dispersed-Electrolyte with High Ionic Conductivity
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  • Dolly Yadav
    Dolly Yadav
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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    Orcidhttps://orcid.org/0000-0003-1322-8074
  • Jung-Hwan Jung
    Jung-Hwan Jung
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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    Orcidhttps://orcid.org/0000-0002-3352-1940
  • Yurim Lee
    Yurim Lee
    Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
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  • Thomas You-Seok Kim
    Thomas You-Seok Kim
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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    Orcidhttps://orcid.org/0009-0006-9392-8431
  • Eunkwang Park
    Eunkwang Park
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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  • Ki-In Choi
    Ki-In Choi
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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  • Jungho Cha
    Jungho Cha
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
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  • Woo-Jin Song*
    Woo-Jin Song
    Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
    Department of Chemical Engineering and Applied Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea
    *Email: [email protected]
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  • Jae-Hak Choi
    Jae-Hak Choi
    Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
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    Orcidhttps://orcid.org/0000-0002-7101-646X
  • Seokgwang Doo
    Seokgwang Doo
    Department of Energy Engineering, Korea Institute of Energy Technology, 72 Unjeong-ro, Naju, Jeonnam 58217, Republic of Korea
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  • Jaewoo Kim*
    Jaewoo Kim
    R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
    *Email: [email protected]
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    Orcidhttps://orcid.org/0000-0003-3472-0180
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Cite this: ACS Materials Lett. 2023, 5, 10, 2648–2655
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https://doi.org/10.1021/acsmaterialslett.3c00538
Published August 30, 2023

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Abstract

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Carbon nanotubes (CNT) are currently used as conductive additives for the electrodes to enhance the capacity of the lithium-ion batteries (LIBs), and we herein for the first time demonstrate the feasibility of boron nitride nanotubes (BNNT) as an electrolyte additive for lithium ion batteries (LIBs). The 0.9 wt % BNNT electrolyte yielded enhanced Li-ion conductivity up to 30% (∼0.87 mS/cm) and a much higher Li-ion transference number (∼0.73) compared to electrolytes without BNNT. The BNNT dispersed electrolyte (1 M LiPF6 in ethylene carbonate/dimethyl carbonate) prepared via sonication serves as a new electrolyte formulation, together with the NCM622//graphite full cell, and exhibits the highest reversible capacities of 153 mAh/g at 1 C and excellent cyclic retention over 500 cycles at high 10 C with a specific capacity of 71.5 mAh/g and a Coulombic efficiency of 99.6% compared to 125.3 mAh/g at 1 C and 40 mAh/g at 10 C with only 97.5% Coulombic efficiency without BNNT, respectively. Overall, we suggest BNNT as a new class of functional electrolyte material that resolves the major limitations of conventional carbonate-based electrolytes and is compatible for different electrolytes/electrode materials aimed at practical implementations for current as well as advanced LIBs.

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Over the last three decades, the materials technology and the manufacturing processes for LIBs have witnessed considerable advancement leading to improved capacities and rendering them capable of powering electric vehicles (EVs). (1−3) In the ongoing pursuit of increasing the energy densities and cycle retention of LIBs, a wide range of promising electrode materials have been tested and commercialized. (4−6) In this regard, carbon nanotubes became a crucial additive for the thick film electrodes increasing the capacity of the LIBs; however, its conductive nature restricted its application as an additive to the separators and/or electrolytes. The electrolytes play an essential role in determining the electrochemical performance of the LIBs. Arguably, one of the biggest challenges is the choice of a suitable electrolyte solution with good ionic conductivity, high Li ion transference, and wide electrochemical stability. The nature of the electrolyte plays a more important role in conventional Li-ion batteries, in determining the nature of solid electrolyte interphase (SEI) formation and regulation of the mass transport of Li+ during the cycling process. Lithium stripping/plating, dendrite growth, effective passivation by SEI, and interference by side reactions are all influenced by the nature of the electrolyte. However, the availability of free Li+ and the medium for transport during the cycling process is a major manipulator that regulates the capacity of the LIBs.

Despite considerable progress made in solid-state electrolytes (SSE) and ionic liquids (IL), conventional liquid electrolytes are still considered the most commonly used electrolytes for LIBs. (7−11) However, due to some inherent limitations, they suffer from long-lasting detrimental loss of capacity of the LIBs. (12,13) In this regard, the electrolyte formulation strategy comes into play, where different additives are added to the conventional electrolytes in order to improve the battery performance. (14−18) Commonly, the electrolyte additives usually comprise of functional molecules that are preferentially involved in the interfacial redox process thereby prior to the electrolytes. (15) They not only improve the interfacial SEI formation but also determine the ionic conductivity and stability of the electrolytes. However, other issues like the reduction in the irreversible capacity, gas generation, thermal stability of Li salt (LiPF6) against organic solvents, and protection of cathode from dissolution and overcharging yet need to be addressed. (17,18) Since not all the desired functions can be achieved by one single additive, hence, binary and ternary additives systems were proposed which definitely adds to the cost and feasibility of the system. (19)

The boron-based additives have been a topic of interest for LIBs. (20,21) Inspired by the promising applications of the hexagonal boron nitrides (h-BN), (22,23) boron nitride nanotubes (BNNT) have been attracted as a viable advanced multifunctional material. (24−26) To date, BNNT has been explored as a protective coating to the separators to reduce the cell short circuit, enhance thermal stability and Li+ conductivity. (25,27) The arrangement of BNNT on the separator results in enhanced Li+ transport, producing a high capacity and negligible change in electrical resistivity. However, incorporating BNNT as an additive into a conventional electrolyte has not been explored. BNNT as an additive would essentially benefit electrolytes with higher ionic conductivity, resulting in boosted Li+ transportation along with resolving thermal issues in LIBs. The fact that the boron centers in BNNT are electron deficient (Lewis acid), they may interact with the oxygen rich electrolyte molecules leading to desolvation of Li+ and hence, improving lithium ion transport through the surface of BNNT as well as inside the tubes. (27)

In this regard, we herein demonstrated, for the first time, the feasibility of BNNT as a multifunctional electrolyte additive to enhance the performance of the conventional LIBs (Scheme 1). BNNT used for the current study displays an open-ended and need-like morphology with a relatively small aspect ratio of 200∼300. (28,29) The SEM image (Figure S1a, Supporting Information) displays the presence of cylindrical nanotube-like morphology with an average length of 5–10 μm. The TEM image of the BNNT (Figure S1b, Supporting Information) displays open-ended cylindrical hollow structures with an outer diameter of 30–50 nm and a length of 5–10 μm in average. The schematic illustration of BNNT dispersion in a 1 M LiPF6 EC/DMC based conventional electrolyte (BNNT-electrolyte) through simple sonication is shown in Scheme 1a. The dispersion of BNNT into electrolytes enhances the confinement effect of the anions at the defect sites. (23−25) In contrast to the conventional electrolytes, Li+ are strongly coordinated with the solvent molecules resulting in comparatively lower capacity and cycle stability also, the Lewis acid interaction between the anions/solvent and the BNNT may facilitate the dissociation of Li+ and accelerate Li+ transport leading to high Li+ transference number. (20) The structural advantage of BNNT for ion transport in fluid media can also be deduced by its hollow and cylindrical geometry (Figure S1b, Supporting Information) that allows fast movement of ions at the surface as well as inside the nanotubes under osmotic, electric, chemical forcing, and their combinations. (26) The Fourier-transform infrared spectroscopy (FTIR, Figure S2, Supporting Information) for the calcinated BNNT (850 °C) conferred the presence of the −OH functional group (3216 cm–1). The −OH functional groups on the BNNT surface serve as interaction sites for the Li-ions providing a channelized pathway for the Li-ion transference during the charge/discharge cycles. (30,31) Hence, BNNT would serve as an excellent electrolyte additive to conventional carbonate electrolytes, bringing multifunctional advantages to LIBs.

Scheme 1

Scheme 1. Design of a BNNT Dispersed Electrolyte, (a) Dispersion of BNNT in Electrolyte through Simple Sonication, and (b) Schematic of NCM/Separator/Graphite Full Cell with BNNT-Dispersed Electrolyte
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The ionic conductivities of BNNT-dispersed electrolytes were measured by electrochemical impedance spectroscopy (EIS), using identical standard stainless-steel disks blocking electrodes at temperatures ranging from −10, 25, and 60 °C, respectively. As shown in Figure 1a, the room temperature ionic conductivities of different BNNT concentrations in 1 M LiPF6 EC/DMC exhibit an upward trend of 0.61, 0.77, 0.80, 0.87, and 0.84 mS/cm with 0.0, 0.5, 0.7, 0.9, and 1.1 wt % of BNNT, respectively. The ionic conductivity of an electrolyte depends on the population of dissociated ion pairs. The Lewis acid sites in the BNNT are assumed to interact with the oxygen of the cyclic carbonates leading to the desolvation of Li+. Hence, the higher ionic conductivity with BNNT could be due to the enhanced movement of free Li+ at the surface and inside the nanotubes and the reduced mobility of the competing anions absorbed at the defect sites in BNNT. Such a phenomenon can be interpreted by the elevated transport channels introduced by BNNT in various transport applications. In addition, the deterioration of LIBs could be minimized with the BNNT electrolytes in terms of ionic conductivity stability with time (Figure 1a). The 0.9 wt % BNNT electrolyte exhibits an improved ionic conductivity of 0.27 mS/cm at −10 °C, which is ∼23% higher than the neat electrolyte (0.22 mS/cm). As expected, BNNT also presents stable and higher ionic conductivity at a high temperature of 60 °C, hence supporting excellent temperature endurance and high Li+ transportation for the BNNT-dispersed-electrolyte (Figure 1b). Comparably, the ionic conductivity for 0.9 wt % BNNT electrolyte is the best among other functional additives dispersed electrolytes prepared and measured under the same conditions and environments (Figure S3, Supporting Information).

Figure 1

Figure 1. (a) Ionic conductivity of x wt % BNNT in 1 M LiPF6 in EC/DMC (1:1 v/v), where x = 0, 0.5, 0.7, 0.9, and 1.1 wt % at 25 °C. (b) Temperature dependent ionic conductivity of the neat and with 0.9 wt % BNNT.

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The Li+ transport efficiency of BNNT electrolytes was also confirmed through their Li+ transference numbers. A symmetric Li (Li//Li) cells with different wt % of BNNT added electrolytes were prepared for measuring tLi+ using the potentiostatic polarization method. (24) The Nyquist plots for the neat and 0.9 wt % BNNT electrolyte are shown in Figure S4. The neat electrolyte displayed tLi+ of ∼0.49 which is in good accordance with the reported literature (tLi+ = 0.47 for 1 M LiPF6 in equivolume EC/DMC). (32) The tLi+ increases with an increase in the wt % of BNNT up to 0.73 for 0.9 wt % BNNT, followed by a further decrease in the tLi+ of 0.70 for 1.1 wt % BNNT (Table 1). Decrease of the tLi+ with higher wt % of BNNT could be partly due to lower amount of electrolyte with increased BNNT content for the equal amount of electrolyte and probable aggregation of BNNT as the concentration is increased in part. The remarkable transport efficiency could be attributed to the structural and surface properties of BNNT that assist the channelized pathway for boosted Li+ transportation imposed by confinement and complexation to the free anions (23) leading to preferential transport of Li+ through the surface and open hollow cylindrical structure.

Table 1. Parameters for the Determination of the Li+ Transference Number with Different wt% of BNNT
BNNT (wt %)R0 (Ω)I0 (μA)Iss (μA)Rss (Ω)tLi+
0 wt %380.4421.9019.30362.590.49
0.5 wt %254.6232.4030.10250.240.66
0.7 wt %221.3539.3037.70218.100.70
0.9 wt %224.2235.6034.00216.230.73
1.1 wt %259.7026.1623.40251.860.70

Further, the electrochemical stability window for BNNT-dispersed-electrolytes was evaluated by cyclic voltammetry (CV) using stainless-steel and Li metal as a working and counter/reference electrode, respectively. The CV curves of the cells using neat and 0.9 wt % BNNT electrolytes show reversible Li/Li+ stripping-plating behavior on steel electrodes between −0.5 and 5.0 V vs Li/Li+ (Figure S5, Supporting Information). The CV curves for 0.9 wt % BNNT added electrolyte (Figure S5a, Supporting Information) exhibited a stable behavior upon repeat cycle in comparison to the neat electrolyte (Figure S5b, Supporting Information). The irreversible moderate oxidation peaks beyond 4.8 V, for 0.9 wt % BNNT electrolyte, demonstrate the electrochemical stability of BNNT added electrolytes with a feasible working window for practical battery applications (inset, Figure S5a, Supporting Information). Indeed, the lower HOMO energy level of EC results in facile oxidation at the cathodic site presenting in lower capacity and lesser cycle stability. (33) However, when BNNT is incorporated into the conventional electrolytes, the boron sites in BNNT interact with the cyclic EC molecules, thereby lowering the chances of electrolyte oxidation, which in turn causes improved capacity and long cycle stability.

In order to experimentally provide the feasibility of practical full cells based on the above assumptions, Li-ion full cell using commercial NCM622 cathode and graphite anode was fabricated with 0.9 wt % BNNT electrolyte (Figure 2). The NCM622//graphite full cell was precycled at a voltage range of 2.7–4.2 V at 0.1 C (Figure 2a). The 0.9 wt % BNNT electrolyte displayed a higher charge capacity (160.3 mAh/g) than the neat electrolyte (152 mAh/g) at 0.1 C. Figure 2b-d shows the temperature dependent electrochemical rate performance of the NCM622//graphite full cell for neat and 0.9 wt % BNNT electrolytes. The rate performance was tested from 0.5C to 15C and back to 1C for neat and 0.9 wt % BNNT electrolyte at 25 °C (Figure 2b) and at 60 °C (Figure 2c). The rate performance at 0.5, 1.0, 5.0, 10, and 15 C for 0.9 wt % BNNT electrolyte at room temperature exhibited specific capacities of 157.9, 153.2, 137.2, 81.2, and 39.5 mAh/g respectively, while the neat electrolyte exhibits 129.4, 125.3, 91.0, 23.13, and 9.7 mAh/g, respectively (Figure 2b). The BNNT electrolytes also exhibited stable and enhanced rate performance at 60 °C with a specific capacity of 116.4, 108.4, 87.99, 65.91, and 40.82 mAh/g, while the neat electrolyte showed lower capacities of 83.9, 71.69, 50.25, 31.13, and 15.5 mAh/g at 0.5, 1.0, 5.0, 10, and 15 C, respectively (Figure 2c).

Figure 2

Figure 2. (a) Precycle voltage profile for NCM622//graphite full cell at 0.1 C, where 1 C = 1.02 mA/cm2 with voltage window of 4.2–2.7 V for Neat and 0.9 wt % BNNT electrolyte, (b) rate performance of NCM//graphite full cell at 25 °C from 0.5 to 15 C for 10 cycles, (c) at 60 °C from 0.5 to 15 C for 5 cycles, (d) at −10 °C from 0.5 to 10 C for five cycles, and (e) galvanostatic cycling of NCM//graphite full cell at 10 C for 500 cycles at 25 °C.

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More importantly, the BNNT electrolyte exhibits a stable rate performance at a freezing temperature of −10 °C (Figure 2d). The 0.9 wt % BNNT electrolyte exhibited 88.6, 38.7, 4.9, and 0.95 mAh/g, while the neat electrolyte exhibited 63.3, 27.1, 4.7, and 0.04 mAh/g at 0.5, 1.0, 5.0, and 10 C, respectively. Further, the cells regained their capacity to 56.1 mAh/g for 0.9 wt % BNNT and 39.2 mAh/g for neat electrolyte at 0.5 C. The lower performance for neat electrolyte could be due to the freezing of the EC at low temperature causing an increase in the ionic resistivity and leading to a rise in the over potential thereby causing a lowering in the ionic conductivity. (34) Also, the low kinetics for Li+ transport induced slow diffusion of Li+ in the active medium that cannot be ignored. In addition, the 0.9 wt % BNNT electrolyte also showed good cycling retention at a high C-rate of 10 C with 71.5 mAh/g specific capacity for over 500 cycles with Coulombic efficiency of 99.6% at 25 °C, while the neat electrolyte showed comparatively lower capacity of 40 mAh/g with only 97.5% Coulombic efficiency under similar conditions (Figure 2e). Hence, it is quite evident that using BNNT as an additive to conventional electrolytes helps in increasing their capacity, cycle retention, varied temperature tolerance, and even stable performance at the higher C-rates.

The postcycle morphology of the electrodes and the separators were imaged by scanning electron microscopy (SEM), to evaluate the effect of BNNT dispersed electrolyte on the performance of the NCM622//graphite full cell. Figure 3 shows the SEM image of the cycled NCM622//graphite full cell at 10 C after 100 cycles. The cycled NCM622 cathode using a neat electrolyte shows little deformation on the surface (Figure 3a) in comparison to the fresh cathode (Figure S6a, Supporting Information). The cycled graphite anode (Figure 3b, 3c) also shows uneven and broken SEI layer formation. The cycled NCM622//graphite full cell using 0.9 wt % BNNT electrolyte shows the presence of BNNT on the NCM surface (Figure 3d, inset and in the cross-section 3e, 3f) along with well-maintained surface even after long cycling experiments (10 C for 100 cycles). Figure 3g–i shows the SEM image of the cycled graphite anode cycled using 0.9 wt % BNNT electrolyte with uniform SEI layer on its surface. The cross section of the anode (Figure 3h, i) also shows the formation of a uniform and porous SEI layer with BNNT deposited on the anode surface as well as embedded in the SEI layer. The presence of BNNT on the surface of the electrode materials is expected to increase the thermal stability of the electrolyte, improve the electrode/electrolyte interface, and the capacity of the LIB. Additionally, the presence of BNNT on the PP separator can also be seen on its surface which expects not only to increase the thermal stability of the separator (Figure S6c, Supporting Information) but also to enhance the ionic conductivity due to directionally oriented to the electrodes (Figure S6d, Supporting Information). The thermal shrinkage of the PP separator procured from the disassembled cells after the cycling experiment was conducted in a convection oven at 120 °C for 1 h. The PP separators with different wt % of BNNT exhibit apparently lesser shrinkage in comparison to the PP separator than that of the neat electrolyte (Figure S7, Supporting Information). As shown in Figure S7, the thermal shrinkage for the PP separator cycled in neat electrolyte was ∼10.5%, which was comparatively higher than the PP separators cycled in BNNT electrolytes with only 5.3, 5.3, 4.7, 4.2, and 2.6% thermal shrinkage for 0.5, 0.7, 0.9, 1.1, and 1.8 wt % BNNT, respectively. Consequently, the introduction of BNNT into conventional electrolytes can remarkably suppress the thermal shrinkage of the PP separator ensuring better battery safety at high temperatures in addition to the increase of the ionic conductivity.

Figure 3

Figure 3. SEM image of disassembled NMC//graphite full cell after 100 cycles at 10 C with neat electrolyte: (a) NCM622 cathode, (b) Graphite anode, (c) cross section of graphite anode, and using 0.9 wt % BNNT electrolyte; (d) NCM622 cathode (inset showing BNNT dispersed on NCM surface); (e, f) cross section of NCM cathode showing presence of BNNT; (g) surface of graphite anode revealing SEI formation; and (h, i) cross section of graphite anode showing the presence of BNNT embedded below the SEI layer. The yellow arrows show the presence of BNNT inside the SEI layer (BNNT attached on the anode surface when the cell first assembled, SEI layer formed during the cycle test).

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For more practical assessment, the 0.9 wt % BNNT electrolyte along with the lithium metal anode and NCM622 cathode was also evaluated. The lithium metal has attracted much attention owing to its high specific capacity (3,860 mAh/g) and low mass density (0.59 g/cm3), however, suffers from poor cycle stability due to the formation of Li-dendrites leading to cell short circuit. (36) The galvanostatic cycling performance for NCM//Li half-cell (Figure S8, Supporting Information) cycled at 0.5 C with a voltage window of 2.7–4.0 V displayed a specific capacity of 175.0 mAh/g with ∼98.7% Coulombic efficiency for 25 cycles, while 153 mAh/g with ∼97.6% Coulombic efficiency for 25 cycles for the neat electrolyte. Furthermore, the LCO//Graphite pouch cells (3 × 3 cm2) for neat and 0.9 wt % BNNT electrolyte were fabricated and precycled at 0.1 C after aging for 36 h (Figure S9, Supporting Information). The precycled LCO//Graphite pouch was cycled at 0.5 C with a voltage window of 4.35 to 2.7 V and exhibited a stable capacity of 15.5 mAh/g retaining 97% Coulombic efficiency even after 300 cycles (Figure S10, Supporting Information). However, the neat electrolyte displayed continuous loss in capacity retaining ∼5.0 mAh/g after 300 cycles with 94.3% Coulombic efficiency at 0.5 C.

Our study strongly suggests that BNNT proves to be an excellent candidate as an electrolyte additive for current LIBs as well as various advanced secondary batteries, including hybrid and all solid-state batteries. Figures S11–S13 shows the X-ray photoelectron spectrometry (XPS) for BNNT before and after exposure to the electrolyte (details in the Supporting Information). After immersing BNNT in the electrolyte for 24 h, followed by centrifugation and vacuum-drying at 100 °C for 24 h, the dried BNNT was then investigated to determine the remaining electrolyte components on the BNNT’s surface. A comparative survey (Figure S11) and the core level spectra (Figure S13) for BNNT after electrolyte exposure displays the presence of F, O, C, N, B, P, and Li with binding energies of F 1s, O 1s, C 1s, N 1s, B 1s, P 2p, and Li 1s at 686.44, 532.71, 284.78, 397.87, 190.3, 134.35, and 55.51 eV, respectively, thereby conferring that the BNNT exhibits electrostatic interactions with the cations, anions as well as the oxygen-rich electrolyte molecules (Figures S11, S12a–g). (35) Further an increase in the carbon and oxygen contents for BNNT after exposure to the electrolyte supported the presence of the electrolyte residue on the BNNT surface. The presence of EC/DMC-related carbon components originates from C–C/C–H (284.78 eV) together with minor contributions from C–O (286.72 eV) and C═O (288.37 eV) species (Figure S13d), which could originate from solvent residues on the BNNT surface. (36) Also, an additional peak a 193.75 eV corresponding to Li–O–B species was also observed for BNNT after electrolyte exposure. (37,38)

The tentative mechanism for Li+ transport for 0.9 wt % BNNT electrolyte is depicted in Scheme 2. The B–N bonds in BNNT are significantly ionic in nature due to the local dipole moment, a typical phenomenon observed in two adjacent heteroatoms. (39,40) This endows BNNT favorable for the electrostatic interactions with the cations, (40) as well as the anions, (39) in the electrolyte thereby providing a pathway for facilitating the Li+ transport. The Lewis acid sites in the BNNT are assumed to interact with the oxygen of the cyclic carbonates, leading to the desolvation of Li+ and hence providing free Li+ responsible for enhanced Li-ion transport. Whereas, the defects sites in BNNT serve as binding sites for the anions, channelizing the transport of Li+ during the charge/discharge process. (20,40) Moreover, due to the structural advantage of the BNNT, (27−29,41) commonly investigated for ion transport in fluid media the open-end hollow cylindrical structure allows the exhohedral and endohedral transport of Li+ through electrostatic interactions. (42−47) Hence, due to the multiple structural benefits, BNNT qualifies as an excellent electrolyte additive for LIBs.

Scheme 2

Scheme 2. Schematic for of the Li+ Transport during Charge and Discharge in (a) Neat Electrolyte and (b) 0.9 wt % BNNT Electrolyte
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In summary, this investigation demonstrates that BNNT dispersed in the conventional electrolytes promotes Li-ion transport efficiency by hindering anion mobility and facilitating Li-ion conduction. Resulting in ∼30% higher ionic conductivity and ∼48% higher tLi+ value than those for the neat electrolyte could offers alleviated polarization, stabilized electrolyte-electrode interfaces, and extended cycle lifespan for current LIBs as well as advanced battery systems. Good capacity retention at a high C-rate (10 C) over 500 cycles while enhancing thermal stability offers the feasibility of BNNT based electrolytes for the high energy density LIBs. Notably, the stable capacity performance at varied temperature conditions (−10 to 60 °C) also offers a solution to the deterioration of LIBs under freezing as well as high temperature conditions, proving its multifunctionality and versatility for future high-performance LIBs. The BNNT electrolytes also show stable and enhanced electrochemical cycle performance for varied cathode (NCM622, LCO) and anode materials (graphite, lithium metal) emphasizing its compatibility with different secondary storage devices. Overall, the above findings further highlight previously unrecognized advantages of BNNT as an electrolyte additive, addressing the major limitations of the conventional carbonate-based electrolyte systems and can provide practical beneficial implementations for the current as well as the advanced battery systems.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmaterialslett.3c00538.

  • Experimental details, ionic conductivities of different filler materials, EIS, CV, SEM images, thermal stability of PP separator, cycle performance of NCM/Li half-cell, voltage profiles and cycle performance of LCO//Graphite pouch cell, and XPS spectra of BNNT before and after electrolyte exposure (PDF)

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Author Information

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  • Corresponding Authors
    • Woo-Jin Song - Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea;  Department of Chemical Engineering and Applied Chemistry, Chungnam National University, Daejeon 34134, Republic of Korea;  Email: [email protected]
    • Jaewoo Kim - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea;  Orcidhttps://orcid.org/0000-0003-3472-0180;  Email: [email protected]
  • Authors
    • Dolly Yadav - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea;  Orcidhttps://orcid.org/0000-0003-1322-8074
    • Jung-Hwan Jung - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea;  Orcidhttps://orcid.org/0000-0002-3352-1940
    • Yurim Lee - Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea
    • Thomas You-Seok Kim - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea;  Orcidhttps://orcid.org/0009-0006-9392-8431
    • Eunkwang Park - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
    • Ki-In Choi - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
    • Jungho Cha - R&D Center, NAiEEL Technology, 6-2 Yuseongdaero 1205, Daejeon 34104, Republic of Korea
    • Jae-Hak Choi - Department of Polymer Science and Engineering, Chungnam National University, Daejeon 34134, Republic of Korea;  Orcidhttps://orcid.org/0000-0002-7101-646X
    • Seokgwang Doo - Department of Energy Engineering, Korea Institute of Energy Technology, 72 Unjeong-ro, Naju, Jeonnam 58217, Republic of Korea
  • Author Contributions

    D.Y. (Dolly Yadav), J.-H.J. (Jung-Hwan Jung), and Y.L. (Yurim Lee) contributed equally to this study. CRediT: Jaewoo Kim conceptualization, funding acquisition, investigation, project administration, writing-review & editing.

  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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This work was financially supported by the R&D Projects Grant No. S3258477 sponsored by the Ministry of SMEs and Startups and Grant No. 20017989 (ATC+ Program) sponsored by the Ministry of Trade, Industry and Energy of Republic of Korea.

References

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    Fan, Xiulin; Chen, Long; Borodin, Oleg; Ji, Xiao; Chen, Ji; Hou, Singyuk; Deng, Tao; Zheng, Jing; Yang, Chongyin; Liou, Sz-Chian; Amine, Khalil; Xu, Kang; Wang, Chunsheng
    Nature Nanotechnology (2018), 13 (8), 715-722CODEN: NNAABX; ISSN:1748-3387. (Nature Research)
    Rechargeable Li-metal batteries using high-voltage cathodes can deliver the highest possible energy densities among all electrochemistries. However, the notorious reactivity of metallic lithium as well as the catalytic nature of high-voltage cathode materials largely prevents their practical application. Here, we report a non-flammable fluorinated electrolyte that supports the most aggressive and high-voltage cathodes in a Li-metal battery. Our battery shows high cycling stability, as evidenced by the efficiencies for Li-metal plating/stripping (99.2%) for a 5 V cathode LiCoPO4 (∼99.81%) and a Ni-rich LiNi0.8Mn0.1Co0.1O2 cathode (∼99.93%). At a loading of 2.0 mAh cm-2, our full cells retain ∼93% of their original capacities after 1,000 cycles. Surface analyses and quantum chem. calcns. show that stabilization of these aggressive chemistries at extreme potentials is due to the formation of a several-nanometer-thick fluorinated interphase.
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    Gond, R.; van Ekeren, W.; Mogensen, R.; Naylor, A. J.; Younesi, R. Non-flammable Liquid Electrolytes for Safe Batteries. Mater. Horiz. 2021, 8, 2913– 2928,  DOI: 10.1039/D1MH00748C
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    Non-flammable liquid electrolytes for safe batteries
    Gond, Ritambhara; van Ekeren, Wessel; Mogensen, Ronnie; Naylor, Andrew J.; Younesi, Reza
    Materials Horizons (2021), 8 (11), 2913-2928CODEN: MHAOBM; ISSN:2051-6355. (Royal Society of Chemistry)
    A review. With continual increments in energy d. gradually boosting the performance of rechargeable alkali metal ion . Li+, Na+, K+ batteries, their safe operation is of growing importance and needs to be considered during their development. This is essential, given the high-profile incidents involving battery fires as portrayed by the media. Such hazardous events result from exothermic chem. reactions occurring between the flammable electrolyte and the electrode material under abusive operating conditions. Some classes of non-flammable org. liq. electrolytes have shown potential towards safer batteries with minimal detrimental effect on cycling and, in some cases, even enhanced performance. This article reviews the state-of-the-art in non-flammable liq. electrolytes for Li-, Na- and K-ion batteries. It provides the reader with an overview of carbonate, ether and phosphate-based org. electrolytes, co-solvated electrolytes and electrolytes with flame-retardant additives as well as highly concd. and locally highly concd. electrolytes, ionic liqs. and inorg. electrolytes. Furthermore, the functionality and purpose of the components present in typical non-flammable mixts. are discussed. Moreover, many non-flammable liq. electrolytes are shown to offer improved cycling stability and rate capability compared to conventional flammable liq. electrolytes.
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    Kim, K.; Ma, H.; Park, S.; Choi, N.-S. Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges. ACS Energy Lett. 2020, 5, 1537– 1553,  DOI: 10.1021/acsenergylett.0c00468
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    19
    Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges
    Kim, Koeun; Ma, Hyunsoo; Park, Sewon; Choi, Nam-Soon
    ACS Energy Letters (2020), 5 (5), 1537-1553CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
    A review. Electrolyte additives have been explored to attain significant breakthroughs in the long-term cycling performance of lithium-ion batteries (LIBs) without sacrificing energy d.; this has been achieved through the development of stable electrode interfacial structures and the elimination of reactive substances. Here we highlight the potential and the challenges raised by studies on electrolyte additives toward addressing the interfacially induced deterioration of high-capacity electrodes with a focus on Ni-rich layered oxides and Si, which are expected to satisfy the growing demands for high-energy-d. batteries. We also discuss issues with the design of electrolyte additives for practical viability. A deep understanding of the roles of existing electrolyte additives depending on their functional groups will aid in the design of functional additive moieties capable of building robust interfacial layers, scavenging undesired reactive species, and suppressing the gas generation that causes safety hazards and shortened lifetimes of LIBs.
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  20. 20
    Zheng, C. Examining the Benefits of Using Boron Compounds in Lithium Batteries: A Comprehensive Review of Literature. Batteries 2022, 8, 187,  DOI: 10.3390/batteries8100187
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    Examining the Benefits of Using Boron Compounds in Lithium Batteries: A Comprehensive Review of Literature
    Zheng, Changlin
    Batteries (Basel, Switzerland) (2022), 8 (10), 187CODEN: BATTAT; ISSN:2313-0105. (MDPI AG)
    A review. Boron and boron compds. have been extensively studied together in the history and development of lithium batteries, which are crucial to decarbonization in the automotive industry and beyond. With a wide examn. of battery components, but a boron-centric approach to raw materials, this review attempts to summarize past and recent studies on the following: which boron compds. are studied in a lithium battery, in which parts of lithium batteries are they studied, what improvements are offered for battery performance, and what improvement mechanisms can be explained. The uniqueness of boron and its extensive application beyond batteries contextualizes the interesting similarity with some studies on batteries. At the end, the article aims to predict prospective trends for future studies that may lead to a more extensive use of boron compds. on a com. scale.
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    Pu, J.; Zhang, K.; Wang, Z.; Li, C.; Zhu, K.; Yao, Y.; Hong, G. Synthesis and Modifications of Boron Nitride Nanomaterials for Electrochemical Energy Storage: From Theory to Application. Adv. Funct. Mater. 2021, 31, 2106315,  DOI: 10.1002/adfm.202106315
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    Synthesis and Modification of Boron Nitride Nanomaterials for Electrochemical Energy Storage: From Theory to Application
    Pu, Jun; Zhang, Kai; Wang, Zhenghua; Li, Chaowei; Zhu, Kaiping; Yao, Yagang; Hong, Guo
    Advanced Functional Materials (2021), 31 (48), 2106315CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)
    A review. As a conventional insulating material, boron nitride (BN) has been mainly investigated in the electronics field. Very recently, with the development of prepn./modification technol. and deeper understanding of the electrochem. mechanisms, BN-based nanomaterials have made significant progress in the field of electrochem. Exploiting the characteristics of BN for advanced electrochem. devices is expected to be a breakthrough that will stimulate a new energy revolution. Owing to its chem. and thermal stability, as well as its high mech. strength, BN can alleviate various inherent problems in electrochem. systems, such as thermal deformation of conventional org. separators, weak solid electrolyte interface layers of metal anodes, and electrocatalyst poisoning. The integration of BN with various electrochem. energy technologies is systematically summarized from the perspectives of material prepn., theor. calcns., and practical applications. Moreover, the challenges and prospects for the future development of BN-based electrochem. are highlighted.
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  22. 22
    Rodrigues, M. -T. F.; Kalaga, K.; Gullapalli, H.; Babu, G.; Reddy, A. L. M.; Ajayan, P. M. Hexagonal Boron Nitride-Based Electrolyte Composite for Li-Ion Battery Operation from Room Temperature to 150 °C. Adv. Energy. Mater. 2016, 6, 1600218,  DOI: 10.1002/aenm.201600218
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    Molaei, Md. J.; Younas, Md.; Rezakazemi, M. Comprehensive Review on Recent Advances in Two-Dimensional (2D) Hexagonal Boron Nitride. ACS Appl. Electron. Mater. 2021, 3, 5165– 5187,  DOI: 10.1021/acsaelm.1c00720
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    A Comprehensive Review on Recent Advances in Two-Dimensional (2D) Hexagonal Boron Nitride
    Molaei, Mohammad Jafar; Younas, Mohammad; Rezakazemi, Mashallah
    ACS Applied Electronic Materials (2021), 3 (12), 5165-5187CODEN: AAEMBP; ISSN:2637-6113. (American Chemical Society)
    A review. Two-dimensional hexagonal boron nitride (2D-hBN) is an emerging 2D material that has received considerable attention due to its exceptional properties including elec. insulation, low dielec. const., easy synthesis, high-temp. stability, corrosion resistance, and chem. stability. 2D-hBN can be integrated with other 2D materials such as graphene in the next-generation of electronic and optoelectronic devices and van der Waals heterostructures. In this review, unique properties of the 2D-hBN are discussed and recent advancements in the synthesis methods such as mech. exfoliation, liq. exfoliation, ion intercalation, chem. vapor deposition, phys. vapor deposition, magnetron sputtering, pulsed laser deposition, ion sputtering deposition, and some more techniques are reviewed. Furthermore, versatile applications of 2D-hBN nanosheets in graphene electronics, tunneling barrier, dielecs., passivation layers, deep UV light sources, single-photon emitters, sensors, and catalysis are critically analyzed. Current challenges and future perspectives for the utilization of 2D-hBN in the next-generation ultrathin electronic devices are discussed.
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    Liu, J.; Cao, D.; Yao, H.; Liu, D.; Zhang, X.; Zhang, Q.; Chen, L.; Wu, S.; Sun, Y.; He, D. Hexagonal Boron Nitride-Coated Polyimide Ion Track Etched Separator with Enhanced Thermal Conductivity and High-Temperature Stability for Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2022, 5, 8639– 8649,  DOI: 10.1021/acsaem.2c01163
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    Rahman, M. M.; Mateti, S.; Cai, Q.; Sultana, I.; Fan, Y.; Wang, X.; Hou, C.; Chen, Y. High Temperature and High-Rate Lithium-Ion Batteries with Boron Nitride Nanotubes Coated Polypropylene Separators. Energy Storage Mater. 2019, 19, 352– 359,  DOI: 10.1016/j.ensm.2019.03.027
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    Jakubinek, M. B.; Kim, K. S.; Kim, M. J.; Martí, A. A.; Pasquali, M. Recent Advances and Perspective on Boron Nitride Nanotubes: From Synthesis to Applications. J. Mater. Res. 2022, 37, 4403– 4418,  DOI: 10.1557/s43578-022-00841-6
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    Recent advances and perspective on boron nitride nanotubes: From synthesis to applications
    Jakubinek, Michael B.; Kim, Keun Su; Kim, Myung Jong; Marti, Angel A.; Pasquali, Matteo
    Journal of Materials Research (2022), 37 (24), 4403-4418CODEN: JMREEE; ISSN:2044-5326. (Springer International Publishing AG)
    A review. Boron nitride nanotubes (BNNTs) are emerging nanomaterials with analogous structures and similarly impressive mech. properties to carbon nanotubes (CNTs), but unique chem. and complimentary multifunctional properties, including higher thermal stability, elec. insulation, optical transparency, neutron absorption capability, and piezoelectricity. Over the past decade, advances in synthesis have made BNNTs more broadly accessible to the nanomaterials and other research communities, removing a major barrier to their utilization and research. Therefore, the field is poised to grow rapidly and see the emergence of BNNT applications ranging from electronics to aerospace materials. A key challenge, that is being gradually overcome, is the development of manufg. processes to make "neat" BNNT materials. This overview highlights the history and current status of the field, providing both an introduction to this Focus Issue-BNNTs: Synthesis to Applications-as well as a perspective on advances, challenges, and opportunities for this emerging material.
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    Chava, B. D.; Wang, Y.; Das, S. Boron Nitride Nanotube–Salt–Water Hybrid: Toward Zero-Dimensional Liquid Water and Highly Trapped Immobile Single Anions Inside One-Dimensional Nanostructures. J. Phys. Chem. C 2021, 125, 14006– 14013,  DOI: 10.1021/acs.jpcc.1c01683
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    Boron Nitride Nanotube-Salt-Water Hybrid: Toward Zero-Dimensional Liquid Water and Highly Trapped Immobile Single Anions Inside One-Dimensional Nanostructures
    Chava, Bhargav Sai; Wang, Yanbin; Das, Siddhartha
    Journal of Physical Chemistry C (2021), 125 (25), 14006-14013CODEN: JPCCCK; ISSN:1932-7447. (American Chemical Society)
    Nanotube-mol.-based hybrid structures, where different chem. species are integrated with the nanotubes either exohedrally (i.e., attached on the outer surface of the nanotubes) or endohedrally (i.e., encapsulated within the nanotubes), have enabled developing novel materials with unprecedented application potential. In this paper, we describe our simulation-driven discovery of an endohedral and noncovalent nanotube-salt-water [boron nitride nanotube (BNNT)-LiTFSI-water] hybrid structure, which forms when a 1 nm diam. BNNT, placed in a large-concn. LiTFSI electrolyte soln., gets filled with periodically repeating and axially sepd. nonoverlapping blocks of the TFSI anion and Li-ion-solvating water. In this hybrid structure, the TFSI anions are in highly trapped immobile state, while the water blocks are in a zero-dimensional configuration and a liq. (noncryst.) state. Furthermore, subjecting the hybrid to elevated temp. or salt-free surrounding has little effect on the structure and properties of this hybrid. This, along with sep. free energy simulations, confirms the most remarkable stability of this nanotube-salt-water hybrid system.
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    Kim, J.; Seo, D.; Yoo, J.; Jeong, W.; Seo, Y.-S.; Kim, J. High Purity and Yield of Boron Nitride Nanotubes Using Amorphous Boron and a Nozzle-Type Reactor. Materials 2014, 7, 5789– 5801,  DOI: 10.3390/ma7085789
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    High purity and yield of boron nitride nanotubes using amorphous boron and a nozzle-type reactor
    Kim, Jaewoo; Seo, Duckbong; Yoo, Jeseung; Jeong, Wanseop; Seo, Young-Soo; Kim, Jaeyong
    Materials (2014), 7 (8), 5789-5801CODEN: MATEG9; ISSN:1996-1944. (MDPI AG)
    Enhancement of the prodn. yield of boron nitride nanotubes (BNNTs) with high purity was achieved using an amorphous boron-based precursor and a nozzle-type reactor. Use of a mixt. of amorphous boron and Fe decreases the milling time for the prepn. of the precursor for BNNTs synthesis, as well as the Fe impurity contained in the B/Fe interdiffused precursor nanoparticles by using a simple purifn. process. We also explored a nozzle-type reactor that increased the prodn. yield of BNNTs compared to a conventional flow-through reactor. By using a nozzle-type reactor with amorphous boron-based precursor, the wt. of the BNNTs sample after annealing was increased as much as 2.5-times with much less impurities compared to the case for the flow-through reactor with the cryst. boron-based precursor. Under the same exptl. conditions, the yield and quantity of BNNTs were estd. as much as ∼70% and ∼1.15 g/batch for the former, while they are ∼54% and 0.78 g/batch for the latter.
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    Kim, J.; Lee, S.; Uhm, Y. R.; Jun, J.; Rhee, C. K.; Kim, G. M. Synthesis and Growth of Boron Nitride Nanotubes by a Ball Milling–Annealing Process. Acta Mater. 2011, 59, 2807– 2813,  DOI: 10.1016/j.actamat.2011.01.019
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    Synthesis and growth of boron nitride nanotubes by a ball milling-annealing process
    Kim, Jaewoo; Lee, Sol; Uhm, Young Rang; Jun, Jiheon; Rhee, Chang Kyu; Kim, Gil Moo
    Acta Materialia (2011), 59 (7), 2807-2813CODEN: ACMAFD; ISSN:1359-6454. (Elsevier Ltd.)
    The synthesis and growth of boron nitride nanotubes (BNNTs) based on ball milling of cryst. boron powder followed by heat treatment were investigated. Fe-based stainless steel (STS) balls and milling vessels were used for milling, and the Fe impurity produced during milling acts as a catalyst for the generation of BNNTs during annealing under a nitrogen environment. Structural deformation of cryst. boron was obsd. for milled boron powder based on X-ray diffraction spectra and electron microscopy images. No chem. reactions of boron with nitrogen occurred during milling, and BNNTs were only synthesized during annealing. The BNNTs produced are basically multi-walled cylindrical- or bamboo-types mixed into nanotube clusters. The diams. of BNNTs are in the range of 50-150 nm, and nos. of the walls are 30-100 with a ∼0.3 nm gap on av. It was obsd. that BN was synthesized from amorphous boron coated onto the surface of the Fe particles. In addn., the types of grown nanotubes could be detd. by the initial shapes of BN clusters on a Fe catalyst particle, which are nanoshells or opened nanocylinders. Yields of BNNTs were strongly dependent on the amorphous structure of the boron particles rather than on the residual cryst. boron particles in the milled samples.
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    Zhang, F.; Nemeth, K.; Bareno, J.; Dogan, F.; Bloom, I. D.; Shaw, L. L. Experimental and Theoretical Investigations of Functionalized Boron Nitride as Electrode Materials for Li-ion Batteries. RSC Adv. 2016, 6, 27901– 27914,  DOI: 10.1039/C6RA03141B
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    Experimental and theoretical investigations of functionalized boron nitride as electrode materials for Li-ion batteries
    Zhang, Fan; Nemeth, Karoly; Bareno, Javier; Dogan, Fulya; Bloom, Ira D.; Shaw, Leon L.
    RSC Advances (2016), 6 (33), 27901-27914CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
    The feasibility of synthesizing functionalized h-BN (FBN) via the reaction between molten LiOH and solid h-BN is studied for the first time and its first ever application as an electrode material in Li-ion batteries is evaluated. D. functional theory (DFT) calcns. are performed to provide mechanistic understanding of the possible electrochem. reactions derived from the FBN. Various materials characterizations reveal that the melt-solid reaction can lead to exfoliation and functionalization of h-BN simultaneously, while electrochem. anal. proves that the FBN can reversibly store charges through surface redox reactions with good cycle stability and coulombic efficiency. DFT calcns. have provided phys. insights into the obsd. electrochem. properties derived from the FBN.
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    Pfaffenhuber, C.; Maier, J. Quantitative estimate of the conductivity of a soggy sand electrolyte: example of (LiClO4, THF):SiO2. J. Phys. Chem. Chem. Phys. 2013, 15, 2050– 2054,  DOI: 10.1039/C2CP43561F
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    Hofmann, A.; Migeot, M.; Thißen, E.; Schulz, M.; Heinzmann, R.; Indris, S.; Bergfeldt, T.; Lei, B.; Ziebert, C.; Hanemann, T. Electrolyte Mixtures Based on Ethylene Carbonate and Dimethyl Sulfone for Li-Ion Batteries with Improved Safety Characteristics. ChemSusChem 2015, 8, 1892– 1900,  DOI: 10.1002/cssc.201500263
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    Electrolyte Mixtures Based on Ethylene Carbonate and Dimethyl Sulfone for Li-Ion Batteries with Improved Safety Characteristics
    Hofmann, Andreas; Migeot, Matthias; Thissen, Eva; Schulz, Michael; Heinzmann, Ralf; Indris, Sylvio; Bergfeldt, Thomas; Lei, Boxia; Ziebert, Carlos; Hanemann, Thomas
    ChemSusChem (2015), 8 (11), 1892-1900CODEN: CHEMIZ; ISSN:1864-5631. (Wiley-VCH Verlag GmbH & Co. KGaA)
    In this study, novel electrolyte mixts. for Li-ion cells are presented with highly improved safety features. The electrolyte formulations are composed of ethylene carbonate/dimethyl sulfone (80:20 wt/wt) as the solvent mixt. and LiBF4, lithium bis(trifluoromethanesulfonyl)azanide, and lithium bis(oxalato)borate as the conducting salts. Initially, the electrolytes are characterized with regard to their phys. properties, their lithium transport properties, and their electrochem. stability. The key advantages of the electrolytes are high flash points of >140 °C, which enhance significantly the intrinsic safety of Li-ion cells contg. these electrolytes. This has been quantified by measurements in an accelerating rate calorimeter. By using the newly developed electrolytes, which are liq. down to T=-10 °C, it is possible to achieve C-rates of up to 1.5 C with >80 % of the initial specific capacity. During 100 cycles in cell tests (graphite||LiNi1/3Co1/3Mn1/3O2), it is proven that the retention of the specific capacity is >98 % of the third discharge cycle with dependence on the conducting salt. The best electrolyte mixt. yields a capacity retention of >96 % after 200 cycles in coin cells.
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    Sun, Z.; Li, F.; Ding, J.; Lin, Z.; Xu, M.; Zhu, M.; Liu, J. High-Voltage and High-Temperature LiCoO2 Operation via the Electrolyte Additive of Electron-Defect Boron Compounds. ACS Energy Lett. 2023, 8, 2478– 2487,  DOI: 10.1021/acsenergylett.3c00324
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    High-Voltage and High-Temperature LiCoO2 Operation via the Electrolyte Additive of Electron-Defect Boron Compounds
    Sun, Zhaoyu; Li, Fangkun; Ding, Jieying; Lin, Zhiye; Xu, Mengqing; Zhu, Min; Liu, Jun
    ACS Energy Letters (2023), 8 (6), 2478-2487CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
    Com. LIBs have the problem of instability interface of electrolyte/cathode at high voltage and high temp. This work reports a novel series of electron-defect boron compds. to construct stable interfaces of LCO/electrolyte. The results of theor. calcn. indicate that compds. of DPD scaffold can win in the competitive oxidn. decompn. for interface regulation. F-rich and B-rich interface is designed by modifying the functional group of DPD scaffold. This strategy of in situ interface design successfully suppresses the dissoln. of harmful transition metal ions and the nucleophilic reaction between electrolyte and cathode. Li/LCO cell can remain stable at high voltage (4.5 V) and high temp. (70 °C) in com. carbonate electrolyte after DPD-F interphase formation. Meanwhile, faster Li+ extn. and insertion kinetics of DPD-F-interface make the Li/LCO cell stable at 4.6 V. Spectral characterizations and theor. calcns. uncover the secret of the forming process of this DPD-F-interface.
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    Li, Q.; Jiao, S.; Luo, L.; Ding, M. S.; Zheng, J.; Cartmell, S. S.; Wang, C.-M.; Xu, K.; Zhang, J.-G.; Xu, W. Wide-Temperature Electrolytes for Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2017, 9, 18826– 18835,  DOI: 10.1021/acsami.7b04099
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    Wide-Temperature Electrolytes for Lithium-Ion Batteries
    Li, Qiuyan; Jiao, Shuhong; Luo, Langli; Ding, Michael S.; Zheng, Jianming; Cartmell, Samuel S.; Wang, Chong-Min; Xu, Kang; Zhang, Ji-Guang; Xu, Wu
    ACS Applied Materials & Interfaces (2017), 9 (22), 18826-18835CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
    Formulating electrolytes with solvents of low f.ps. and high dielec. consts. is a direct approach to extend the service-temp. range of lithium (Li)-ion batteries (LIBs). In this study, we report such wide-temp. electrolyte formulations by optimizing the ethylene carbonate (EC) content in the ternary solvent system of EC, propylene carbonate (PC), and Et Me carbonate (EMC) with LiPF6 salt and CsPF6 additive. An extended service-temp. range from -40 to 60 °C was obtained in LIBs with lithium nickel cobalt aluminum oxide (LiNi0.80Co0.15Al0.05O2, NCA) as cathode and graphite as anode. The discharge capacities at low temps. and the cycle life at room temp. and elevated temps. were systematically investigated together with the ionic cond. and phase-transition behaviors. The most promising electrolyte formulation was identified as 1.0 M LiPF6 in EC-PC-EMC (1:1:8 by wt) with 0.05 M CsPF6, which was demonstrated in both coin cells of graphite‖NCA and 1 Ah pouch cells of graphite‖LiNi1/3Mn1/3Co1/3O2. This optimized electrolyte enables excellent wide-temp. performances, as evidenced by the high capacity retention (68%) at -40 °C and C/5 rate, significantly higher than that (20%) of the conventional LIB electrolyte, and the nearly identical stable cycle life as the conventional LIB electrolyte at room temp. and elevated temps. up to 60 °C.
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    Silva, W. M.; Ribeiro, H.; Taha-Tijerina, J. J. Potential Production of Theranostic Boron Nitride Nanotubes (64Cu-BNNTs) Radiolabeled by Neutron Capture. Nanomaterials 2021, 11, 2907,  DOI: 10.3390/nano11112907
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    Potential Production of Theranostic Boron Nitride Nanotubes (64Cu-BNNTs) Radiolabeled by Neutron Capture
    Silva, Wellington Marcos; Ribeiro, Helio; Taha-Tijerina, Jose Jaime
    Nanomaterials (2021), 11 (11), 2907CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
    In this work, the radioisotope 64Cu was obtained from copper (II) chloride dihydrate in a nuclear research reactor by neutron capture, (63Cu(n, γ)64Cu), and incorporated into boron nitride nanotubes (BNNTs) using a solvothermal process. The produced 64Cu-BNNTs were analyzed by TEM, MEV, FTIR, XDR, XPS and gamma spectrometry, with which it was possible to observe the formation of 64Cu nanoparticles, with sizes of up to 16 nm, distributed through nanotubes. The synthesized of 64Cu nanostructures showed a pure photoemission peak of 511 keV, which is characteristic of gamma radiation. This type of emission is desirable for photon emission tomog. (PET scan) image acquisition, as well as its use in several cancer treatments. Thus, 64Cu-BNNTs present an excellent alternative as theranostic nanomaterials that can be used in diagnosis and therapy by different techniques used in nuclear medicine.
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    Dietrich, P. M.; Gehrlein, J.; Maibach, j.; Thissen, A. Probing Lithium-Ion Battery Electrolytes with Laboratory Near-Ambient Pressure XPS. Crystals 2020, 10, 1056,  DOI: 10.3390/cryst10111056
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    Probing lithium-ion battery electrolytes with laboratory near-ambient pressure XPS
    Dietrich, Paul M.; Gehrlein, Lydia; Maibach, Julia; Thissen, Andreas
    Crystals (2020), 10 (11), 1056CODEN: CRYSBC; ISSN:2073-4352. (MDPI AG)
    In this article, we present Near Ambient Pressure (NAP)-XPS results from model and com. liq. electrolytes for lithium-ion battery prodn. using an automated lab. NAP-XPS system. The electrolyte solns. were (i) LiPF6 in EC/DMC (LP30) as a typical com. battery electrolyte and (ii) LiTFSI in PC as a model electrolyte. We analyzed the LP30 electrolyte soln., first in its vapor and liq. phase to compare individual core-level spectra. In a second step, we immersed a V2O5 crystal as a model cathode material in this LiPF6 soln. Addnl., the LiTFSI electrolyte model system was studied to compare and verify our findings with previous NAP-XPS data. Photoelectron spectra recorded at pressures of 2-10 mbar show significant chem. differences for the different lithium-based electrolytes. We show the enormous potential of lab. NAP-XPS instruments for investigations of solid-liq. interfaces in electrochem. energy storage systems at elevated pressures and illustrate the simplicity and ease of the used exptl. setup (EnviroESCA).
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    Matsoso, J. B.; Vuillet-a-Ciles, V.; Bois, L.; Toury, B.; Journet, C. Improving Formation Conditions and Properties of hBN Nanosheets Through BaF2-assisted Polymer Derived Ceramics (PDCs) Technique. Nanomaterials 2020, 10, 443,  DOI: 10.3390/nano10030443
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    Improving formation conditions and properties of hBN nanosheets through BaF2-assisted polymer derived ceramics (PDCs) technique
    Matsoso, Boitumelo J.; Vuillet-a-Ciles, Victor; Bois, Laurence; Toury, Berangere; Journet, Catherine
    Nanomaterials (2020), 10 (3), 443CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
    Hexagonal boron nitrite (hBN) is an attractive material for many applications such as in electronics as a complement to graphene, in anti-oxidn. coatings, light emitters, etc. However, the synthesis of high-quality hBN at cost-effective conditions is still a great challenge. Thus, this work reports on the synthesis of large-area and cryst. hBN nanosheets via the modified polymer derived ceramics (PDCs) process. The addn. of both the BaF2 and Li3N, as melting-point redn. and crystn. agents, resp., led to the prodn. of hBN powders with excellent physicochem. properties at relatively low temps. and atm. pressure conditions. For instance, XRD, Raman, and XPS data revealed improved crystallinity and quality at a decreased formation temp. of 1200°C upon the addn. of 5 wt% of BaF2. Moreover, morphol. detn. illustrated the formation of multi-layered nanocryst. and well-defined shaped hBN powders with crystal sizes of 2.74-8.41 ± 0.71μm in diam. Despite the compromised thermal stability, as shown by the ease of oxidn. at high temps., this work paves way for the prodn. of large-scale and high-quality hBN crystals at a relatively low temp. and atm. pressure conditions.
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    Charles-Blin, Y.; Nemoto, K.; Zettsu, N.; Teshima, K. Effects of a Solid Electrolyte Coating on the Discharge Kinetics of a LiCoO2 Electrode: Mechanism and Potential Applications. J. Mater. Chem. A 2020, 8, 20979– 20986,  DOI: 10.1039/D0TA05656A
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    Effects of a solid electrolyte coating on the discharge kinetics of a LiCoO2 electrode: mechanism and potential applications
    Charles-Blin, Youn; Nemoto, Kazune; Zettsu, Nobuyuki; Teshima, Katsuya
    Journal of Materials Chemistry A: Materials for Energy and Sustainability (2020), 8 (40), 20979-20986CODEN: JMCAET; ISSN:2050-7496. (Royal Society of Chemistry)
    The application of a Li+-conductive amorphous Li2B4O7 coating on a LiCoO2 electrode enhanced its discharge kinetics by increasing the local concn. of Li+ at the surface of LiCoO2 particles. The origin of internal resistance in Li+ intercalation steps was elucidated by electrochem. impedance spectroscopy (EIS)-based characterization of discharge kinetics for states of charges of 0, 50, and 100%, while the activation energies of intercalation steps were detd. from EIS data collected at different temps. (-10, 0, 20, and 40°C). The activation energy of Li+ desolvation was smaller than that previously reported for bare LiCoO2 particles, which suggested that the significant changes in kinetics assocd. with polarization mitigation were due to the Li+ exchange reaction (Li+ adsorption and diffusion processes) on the surface of LiCoO2 particles. Finally, C-rate capability tests performed at -10°C revealed that the capacity retention of the electrode comprising Li2B4O7-coated LiCoO2 particles exceeded that of the electrode comprising bare LiCoO2 particles (45% vs. 18%, resp.).
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    Zhang, D.; Zhang, S.; Yapici, N.; Oakley, R.; Sharma, S.; Parashar, V.; Yap, Y. K. Emerging Applications of Boron Nitride Nanotubes in Energy Harvesting, Electronics, and Biomedicine. ACS Omega 2021, 6, 20722– 20728,  DOI: 10.1021/acsomega.1c02586
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    Emerging Applications of Boron Nitride Nanotubes in Energy Harvesting, Electronics, and Biomedicine
    Zhang, Dongyan; Zhang, Siqi; Yapici, Nazmiye; Oakley, Rodney; Sharma, Sambhawana; Parashar, Vyom; Yap, Yoke Khin
    ACS Omega (2021), 6 (32), 20722-20728CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
    A review. Boron nitride nanotubes (BNNTs) are structurally and mech. similar to carbon nanotubes (CNTs). In contrast, BNNTs exhibit unique properties for being elec. insulating and optically transparent due to the polarized boron nitride bonds. All these properties have prevented the use of BNNTs for energy harvesting and electronic devices for more than 25 years. During the past few years, researchers have started to demonstrate a series of novel applications of BNNTs based on unique properties not found on CNTs. For example, these novel applications include osmotic power harvesting using the charged inner surfaces of BNNTs, room-temp. single-electron transistors using insulating BNNTs as the tunneling channels, high-brightness fluorophores that can be 1000-times brighter than regular dyes, and transistors based on Tellurium at. chains filled inside BNNTs. We have reviewed some of these emerging applications and provided our perspective for future work.
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    Cheng, X.-B.; Zhang, R.; Zhao, C.-Z.; Zhang, Q. Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review. Chem. Rev. 2017, 117, 10403– 10473,  DOI: 10.1021/acs.chemrev.7b00115
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    Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review
    Cheng, Xin-Bing; Zhang, Rui; Zhao, Chen-Zi; Zhang, Qiang
    Chemical Reviews (Washington, DC, United States) (2017), 117 (15), 10403-10473CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)
    A review is presented. The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-d. energy storage devices in our modern and technol.-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and tech. challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quant. models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theor. understanding and anal., recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applications is included. A general conclusion and a perspective on the current limitations and recommended future research directions of lithium metal batteries are presented. The review concludes with an attempt at summarizing the theor. and exptl. achievements in lithium metal anodes and endeavors to realize the practical applications of lithium metal batteries.
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    Choi, K.-I.; Yadav, D.; Jung, J.; Park, E.; Lee, K.-M.; Kim, T.; Kim, J. Noble Metal Nanoparticles Decorated Boron Nitride Nanotubes for Efficient and Selective Low-Temperature Catalytic Reduction of Nitric Oxide with Carbon Monoxide. ACS Appl. Mater. Interfaces 2023, 15, 10670– 10678,  DOI: 10.1021/acsami.2c20985
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    Noble Metal Nanoparticles Decorated Boron Nitride Nanotubes for Efficient and Selective Low-Temperature Catalytic Reduction of Nitric Oxide with Carbon Monoxide
    Choi, Ki-In; Yadav, Dolly; Jung, Junghwan; Park, Eunkwang; Lee, Kyung-Min; Kim, Taejin; Kim, Jaewoo
    ACS Applied Materials & Interfaces (2023), 15 (8), 10670-10678CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
    Parallel to CO2 emission, NOx emission has become one of the menacing problems that seek a simple, durable, and high-efficiency deNOx catalyst. Herein, the authors demonstrated simple syntheses of Pt group metal nanoparticle-decorated f-BNNT (PGM = Pd, Pt, and Rh, and f-BNNT stands for -OH-functionalized B nitride nanotubes) as a catalyst for efficient and selective redn. of NO by CO at low-temp. conditions. PGM/f-BNNT with a low amt. of noble metal nanoparticles (0.7-0.8%) presents very efficient catalytic activity for NO redn. as well as CO oxidn. during their removal process. The removal efficiencies of NO and CO with Pd/f-BNNT, Pt/f-BNNT, and Rh/f-BNNT catalysts were studied under various temps., flow rates, and reaction times, resp. For most cases, NO catalytic redn. with CO reaction was >99% at a temp. as low as ~ 200°. The catalyst robustness and efficiency were also verified by presenting almost 100% conversion of NO using a Rh/f-BNNT catalyst, which was aged under humid air at 600 and 700° for 24 h, resp. The synergic effect of the catalytic efficacy of the well-dispersed noble metal nanoparticles and the excellent surface properties of BNNT are reasons for the high selectivity and catalytic property at a low temp. The noble metal nanoparticle-decorated f-BNNT catalysts are possible to save expensive PGM catalysts, such as Pt, Pd, and Rd, ≤100 times while presenting similar or better catalytic performance for simultaneous NO and CO removals.
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    Li, Y.; Zhang, L.; Sun, Z.; Gao, G.; Lu, S.; Zhu, M.; Zhang, Y.; Jia, Z.; Xiao, C.; Bu, H.; Xi, K.; Ding, S. Hexagonal Boron Nitride Induces Anion Trapping in a Polyethylene Oxide Based Solid Polymer Electrolyte for Lithium Dendrite Inhibition. J. Mater. Chem. A 2020, 8, 9579– 9589,  DOI: 10.1039/D0TA03677C
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    Hexagonal boron nitride induces anion trapping in a polyethylene oxide based solid polymer electrolyte for lithium dendrite inhibition
    Li, Yuhan; Zhang, Libo; Sun, Zongjie; Gao, Guoxin; Lu, Shiyao; Zhu, Min; Zhang, Yanfeng; Jia, Zhiyu; Xiao, Chunhui; Bu, Huaitian; Xi, Kai; Ding, Shujiang
    Journal of Materials Chemistry A: Materials for Energy and Sustainability (2020), 8 (19), 9579-9589CODEN: JMCAET; ISSN:2050-7496. (Royal Society of Chemistry)
    Here a hexagonal boron nitride (h-BN)-polyethylene oxide composite polymer electrolyte is prepd. via a convenient casting method, which shows high mech. strength. Meanwhile, the electrochem. properties (electrochem. window and lithium ion transference no.) are enhanced but the ionic cond. of the h-BN composite electrolyte is decreased after adding h-BN. D. functional theory (DFT) calcn. results show that a stronger binding effect is obsd. between TFSI- and BN, compared to that between Li+ and BN. Mol. dynamics (MD) simulations are also utilized to study the mechanism behind the enhanced Li ion diffusion by h-BN addn. Li+ diffusion in PEO/LiTFSI/BN is lower than that in the PEO/LiTFSI system, but the diffusion of TFSI- exhibits a more significant decline rate in the presence of BN. This indicates that the presence of BN suppresses anion motion and enhances selectivity in Li+ transport. Thus, the PEO/LiTFSI/h-BN composite electrolyte exhibits higher Li ion cond. but lower anion diffusivity than the PEO/LiTFSI system. Hence the h-BN composite polymer electrolyte in a Li/Li sym. battery provides a long cycling time of 430 h at 0.2 mA cm-2. A Li metal/LiFePO4 full battery with the PEO/LiTFSI/h-BN composite electrolyte also works more efficiently for long-term cycling (140 cycles) than a filler-free PEO based electrolyte (39 cycles).
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    Cetindag, S.; Tiwari, B.; Zhang, D.; Yap, Y. K.; Kim, S.; Shan, J. Surface-Charge Effects on the Electro-Orientation of Insulating Boron-Nitride Nanotubes in Aqueous Suspension. J. Colloid Interface Sci. 2017, 505, 1185– 1192,  DOI: 10.1016/j.jcis.2017.05.073
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    Surface-charge effects on the electro-orientation of insulating boron-nitride nanotubes in aqueous suspension
    Cetindag, Semih; Tiwari, Bishnu; Zhang, Dongyan; Yap, Yoke Khin; Kim, Sangil; Shan, Jerry W.
    Journal of Colloid and Interface Science (2017), 505 (), 1185-1192CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)
    The alignment of hexagonal boron-nitride nanotubes (BNNTs) in aq. KCl solns. under spatially uniform elec. fields was examd. exptl., using direct optical visualization to probe the orientation dynamics of individual BNNTs for different elec.-field frequencies. Different from most previously studied nanowires and nanotubes, BNNTs are wide-bandgap materials which are essentially insulating at room temp. The authors analyze the electro-orientation of BNNTs in the general context of polarizable cylindrical particles in liq. suspensions, whose behavior can fall into different regimes, including alignment due to Maxwell-Wagner induced dipoles at high frequencies, and alignment due to fluid motion of the elec. double layer around the particles at lower frequencies. For BNNTs, the variation of the crossover frequencies in the electro-orientation spectra was studied in electrolytes of different cond. The effect of BNNT surface charge on electro-orientation was further studied by changing the pH of the aq. soln. The authors find that the elec.-field alignment of the BNNTs in the low-frequency regime is assocd. with the charging and motion of the elec. double layer around the particle. However, as BNNTs are non-conducting particles, the reasons for the formation of the elec. double layer are likely to be different than that of conducting particles. The authors discuss two possible mechanisms for the double-layer formation and alignment of 1D dielec. particles, and make comparison to those for the more commonly studied conducting particles.
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    Zuo, K.; Zhang, X.; Huang, X.; Oliveira, E. F.; Guo, H.; Zhai, T.; Wang, W.; Alvarez, P. J. J.; Elimelech, M.; Ajayan, P. K.; Lou, J.; Li, Q. Ultrahigh Resistance of Hexagonal Boron Nitride to Mineral Scale Formation. Nat. Commun. 2022, 13, 4523,  DOI: 10.1038/s41467-022-32193-4
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    Ultrahigh resistance of hexagonal boron nitride to mineral scale formation
    Zuo, Kuichang; Zhang, Xiang; Huang, Xiaochuan; Oliveira, Eliezer F.; Guo, Hua; Zhai, Tianshu; Wang, Weipeng; Alvarez, Pedro J. J.; Elimelech, Menachem; Ajayan, Pulickel M.; Lou, Jun; Li, Qilin
    Nature Communications (2022), 13 (1), 4523CODEN: NCAOBW; ISSN:2041-1723. (Nature Portfolio)
    Abstr.: Formation of mineral scale on a material surface has profound impact on a wide range of natural processes as well as industrial applications. However, how specific material surface characteristics affect the mineral-surface interactions and subsequent mineral scale formation is not well understood. Here we report the superior resistance of hexagonal boron nitride (hBN) to mineral scale formation compared to not only common metal and polymer surfaces but also the highly scaling-resistant graphene, making hBN possibly the most scaling resistant material reported to date. Exptl. and simulation results reveal that this ultrahigh scaling-resistance is attributed to the combination of hBNs atomically-smooth surface, in-plane at. energy corrugation due to the polar boron-nitrogen bond, and the close match between its interat. spacing and the size of water mols. The latter two properties lead to strong polar interactions with water and hence the formation of a dense hydration layer, which strongly hinders the approach of mineral ions and crystals, decreasing both surface heterogeneous nucleation and crystal attachment.
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    Siria, A.; Poncharal, P.; Biance, A. L.; Fulcrand, R.; Blasé, X.; Purcell, S. T.; Bocquet, L. Giant Osmotic Energy Conversion Measured in a Single Transmembrane Boron Nitride Nanotube. Nature 2013, 494, 455– 458,  DOI: 10.1038/nature11876
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    Giant osmotic energy conversion measured in a single transmembrane boron nitride nanotube
    Siria, Alessandro; Poncharal, Philippe; Biance, Anne-Laure; Fulcrand, Remy; Blase, Xavier; Purcell, Stephen T.; Bocquet, Lyderic
    Nature (London, United Kingdom) (2013), 494 (7438), 455-458CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
    New models of fluid transport are expected to emerge from the confinement of liqs. at the nanoscale, with potential applications in ultrafiltration, desalination and energy conversion. Nevertheless, advancing our fundamental understanding of fluid transport on the smallest scales requires mass and ion dynamics to be ultimately characterized across an individual channel to avoid averaging over many pores. A major challenge for nanofluidics thus lies in building distinct and well-controlled nanochannels, amenable to the systematic exploration of their properties. Here we describe the fabrication and use of a hierarchical nanofluidic device made of a boron nitride nanotube that pierces an ultrathin membrane and connects two fluid reservoirs. Such a transmembrane geometry allows the detailed study of fluidic transport through a single nanotube under diverse forces, including elec. fields, pressure drops and chem. gradients. Using this device, we discover very large, osmotically induced elec. currents generated by salinity gradients, exceeding by two orders of magnitude their pressure-driven counterpart. We show that this result originates in the anomalously high surface charge carried by the nanotube's internal surface in water at large pH, which we independently quantify in conductance measurements. The nano-assembly route using nanostructures as building blocks opens the way to studying fluid, ionic and mol. transport on the nanoscale, and may lead to biomimetic functionalities. Our results furthermore suggest that boron nitride nanotubes could be used as membranes for osmotic power harvesting under salinity gradients.
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    Kim, D.; Liu, X.; Yu, B.; Mateti, S.; O’Dell, L. A.; Rong, Q.; Chen, Y. Amine-Functionalized Boron Nitride Nanosheets: A New Functional Additive for Robust, Flexible Ion Gel Electrolyte with High Lithium-Ion Transference Number. Adv. Funct. Mater. 2020, 30, 1910813,  DOI: 10.1002/adfm.201910813
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    Amine-Functionalized Boron Nitride Nanosheets: A New Functional Additive for Robust, Flexible Ion Gel Electrolyte with High Lithium-Ion Transference Number
    Kim, Donggun; Liu, Xin; Yu, Baozhi; Mateti, Srikanth; O'Dell, Luke A.; Rong, Qiangzhou; Chen, Ying
    Advanced Functional Materials (2020), 30 (15), 1910813CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)
    Ion gel electrolytes show great potential in solid-state batteries attributed to their outstanding characteristics. However, because of the strong ionic nature of ionic liqs., ion gel electrolytes generally exhibit low lithium-ion transference no., limiting its practical application. Amine-functionalized boron nitride (BN) nanosheets (AFBNNSs) are used as an additive into ion gel electrolytes for improving their ion transport properties. The AFBNNSs-ion gel shows much improved mech. strength and thermal stability. The lithium-ion transference no. is increased from 0.12-0.23 due to AFBNNS addn. More importantly, for the first time, NMR anal. reveals that the amine groups on the BN nanosheets have strong interaction with the bis(trifluoromethanesulfonyl)imide anions, which significantly reduces the anion mobility and consequently increases lithium-ion mobility. Battery cells using the optimized AFBNNSs-ion gel electrolyte exhibit stable lithium deposition and excellent electrochem. performance. A LiFePO4|Li cell retains 92.2% of its initial specific capacity after the 60th cycle while the cell without AFBNNSs-gel electrolyte only retains 53.5%. The results not only demonstrate a new strategy to improve lithium-ion transference no. in ionic liq. electrolytes, but also open up a potential avenue to achieve solid-state lithium metal batteries with improved performance.
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    Liu, W.; Lee, S. W.; Lin, D.; Shi, F.; Wang, S.; Sendek, A. D.; Cui, Y. Enhancing Ionic Conductivity in Composite Polymer Electrolytes with Well-Aligned Ceramic Nanowires. Nat. Energy 2017, 2, 17035,  DOI: 10.1038/nenergy.2017.35
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    Enhancing ionic conductivity in composite polymer electrolytes with well-aligned ceramic nanowires
    Liu, Wei; Lee, Seok Woo; Lin, Dingchang; Shi, Feifei; Wang, Shuang; Sendek, Austin D.; Cui, Yi
    Nature Energy (2017), 2 (5), 17035CODEN: NEANFD; ISSN:2058-7546. (Nature Publishing Group)
    In contrast to conventional org. liq. electrolytes that have leakage, flammability and chem. stability issues, solid electrolytes are widely considered as a promising candidate for the development of next-generation safe lithium-ion batteries. In solid polymer electrolytes that contain polymers and lithium salts, inorg. nanoparticles are often used as fillers to improve electrochem. performance, structure stability, and mech. strength. However, such composite polymer electrolytes generally have low ionic cond. Here we report that a composite polymer electrolyte with well-aligned inorg. Li+-conductive nanowires exhibits an ionic cond. of 6.05 × 10-5 S cm-1 at 30 oC, which is one order of magnitude higher than previous polymer electrolytes with randomly aligned nanowires. The large cond. enhancement is ascribed to a fast ion-conducting pathway without crossing junctions on the surfaces of the aligned nanowires. Moreover, the long-term structural stability of the polymer electrolyte is also improved by the use of nanowires.
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  1. Numan Yanar, Thomas You-Seok Kim, Junghwan Jung, Duy Khoe Dinh, Ki-in Choi, Arni G. Pornea, Dolly Yadav, Zahid Hanif, Eunkwang Park, Jaewoo Kim. Boron Nitride Nanotube-Aligned Electrospun PVDF Nanofiber-Based Composite Films Applicable to Wearable Piezoelectric Sensors. ACS Applied Nano Materials 2024, 7 (10) , 11715-11726. https://doi.org/10.1021/acsanm.4c01296
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  • Abstract

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    Scheme 1

    Scheme 1. Design of a BNNT Dispersed Electrolyte, (a) Dispersion of BNNT in Electrolyte through Simple Sonication, and (b) Schematic of NCM/Separator/Graphite Full Cell with BNNT-Dispersed Electrolyte
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    Figure 1

    Figure 1. (a) Ionic conductivity of x wt % BNNT in 1 M LiPF6 in EC/DMC (1:1 v/v), where x = 0, 0.5, 0.7, 0.9, and 1.1 wt % at 25 °C. (b) Temperature dependent ionic conductivity of the neat and with 0.9 wt % BNNT.

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    Figure 2

    Figure 2. (a) Precycle voltage profile for NCM622//graphite full cell at 0.1 C, where 1 C = 1.02 mA/cm2 with voltage window of 4.2–2.7 V for Neat and 0.9 wt % BNNT electrolyte, (b) rate performance of NCM//graphite full cell at 25 °C from 0.5 to 15 C for 10 cycles, (c) at 60 °C from 0.5 to 15 C for 5 cycles, (d) at −10 °C from 0.5 to 10 C for five cycles, and (e) galvanostatic cycling of NCM//graphite full cell at 10 C for 500 cycles at 25 °C.

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    Figure 3

    Figure 3. SEM image of disassembled NMC//graphite full cell after 100 cycles at 10 C with neat electrolyte: (a) NCM622 cathode, (b) Graphite anode, (c) cross section of graphite anode, and using 0.9 wt % BNNT electrolyte; (d) NCM622 cathode (inset showing BNNT dispersed on NCM surface); (e, f) cross section of NCM cathode showing presence of BNNT; (g) surface of graphite anode revealing SEI formation; and (h, i) cross section of graphite anode showing the presence of BNNT embedded below the SEI layer. The yellow arrows show the presence of BNNT inside the SEI layer (BNNT attached on the anode surface when the cell first assembled, SEI layer formed during the cycle test).

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    Scheme 2

    Scheme 2. Schematic for of the Li+ Transport during Charge and Discharge in (a) Neat Electrolyte and (b) 0.9 wt % BNNT Electrolyte
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      ACS Energy Letters (2017), 2 (11), 2563-2575CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
      A review. The continued search for routes to improve the power and energy d. of lithium ion batteries for elec. vehicles and consumer electronics has resulted in significant innovation in all cell components, particularly in electrode materials design. In this Review, we highlight an often less noted route to improving energy d.: increasing the Li+ transference no. of the electrolyte. Turning to Newman's original lithium ion battery models, we demonstrate that electrolytes with modestly higher Li+ transference nos. compared to traditional carbonate-based liq. electrolytes would allow higher power densities and enable faster charging (e.g., >2C), even if their cond. was substantially lower than that of conventional electrolytes. Most current research in high transference no. electrolytes (HTNEs) focuses on ceramic electrolytes, polymer electrolytes, and ionomer membranes filled with nonaq. solvents. We highlight a no. of the challenges limiting current HTNE systems and suggest addnl. work on promising new HTNE systems, such as "solvent-in-salt" electrolytes, perfluorinated solvent electrolytes, nonaq. polyelectrolyte solns., and solns. contg. anion-decorated nanoparticles.
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      Revealing the Impact of Fast Charge Cycling on the Thermal Safety of Lithium-Ion Batteries
      Zhang, Guangxu; Wei, Xuezhe; Chen, Siqi; Zhu, Jiangong; Han, Guangshuai; Wang, Xueyuan; Dai, Haifeng
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      The safety of the degraded lithium-ion batteries has an essential impact on second life application. This study systematically investigates the thermal safety changes of lithium-ion batteries after deep aging under the fast charge aging path and reveals the degrdn. mechanisms caused by fast charge cycling. Lithium plating is the primary degrdn. mechanism, which thickens the solid electrolyte interface film, causes the loss of active lithium and electrolyte, and leads to a significant increase in impedance and a dramatic decrease in capacity. Therefore, compared with the fresh cells, the heat generation rate increases, while the total heat generation is reduced for aged cells. Besides, the thickened solid electrolyte interface film has lower thermal stability, decreasing the self-heating temp. for aged cells. Furthermore, thermal runaway results of partial cells prove that fast charge cycling reduces the thermal stability of the anode, which further proves that the thermal runaway-triggering temp. decrease is the result of the combination of the anode-electrolyte and anode-cathode reactions. Moreover, fast charge cycling reduces the lithium plating potential upon overcharging, which leads to the occurrence of side reactions in advance, creating the ratio of side reaction heat increase of aged cells for thermal runaway triggering. In addn., the loss of active materials reduces the max. temp. and max. temp. rise rate of the aged cell. The findings can provide refs. for battery safety management system optimization and safer battery screening.
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      Sun, S.; Wang, J.; Chen, X.; Ma, Q.; Wang, Y.; Yang, K.; Yao, X.; Yang, Z.; Liu, J.; Xu, H. Thermally Stable and Dendrite-Resistant Separators toward Highly Robust Lithium Metal Batteries. Adv. Energy. Mater. 2022, 12, 2202206,  DOI: 10.1002/aenm.202202206
      13
      Thermally Stable and Dendrite-Resistant Separators toward Highly Robust Lithium Metal Batteries
      Sun, Shiyi; Wang, Jianan; Chen, Xin; Ma, Qianyue; Wang, Yanyao; Yang, Kai; Yao, Xuhui; Yang, Zhipeng; Liu, Jianwei; Xu, Hao; Cai, Qiong; Zhao, Yunlong; Yan, Wei
      Advanced Energy Materials (2022), 12 (41), 2202206CODEN: ADEMBC; ISSN:1614-6840. (Wiley-Blackwell)
      High-level safety is of vital importance to the continuous pursuit of high-energy-d. batteries in the increasingly electrified world. The thermal instability and dendrite-induced issues of conventional polypropylene (PP) separators often cause internal short circuits and thermal runaway in batteries. Herein, a thermally stable and dendrite-resistant separator (F-PPTA@PP) is constructed using a dual-functional and easy-to-commercialize design strategy of thermally safe poly-p-phenylene-terephthamide nanofibers and plasma-induced lithiophilic fluorine-contg. groups. In situ thermal monitoring, in situ optical observation, and multiphysics simulation demonstrate that F-PPTA@PP can suppress thermal shrinkage of the separator and the formation of hotspots, and also promote uniform lithium deposition. Subsequently, lithium metal batteries are assembled, featuring an initial capacity of 194.1 mAh g-1 at 0.5 C with a low-capacity attenuation of 0.02% per cycle over 1000 cycles. When operating under extreme conditions, i.e., -10 and 100°C, ultrafast charging/discharging rates up to 30 C, lean electrolyte (2.4μL mg-1)/high mass-loading (10.77 mg cm-2) or lithium-sulfur batteries, F-PPTA@PP separator still enables competitive electrochem. performance, highlighting its plausible processing scalability for high-safety energy storage systems.
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      Chang, Z.; Qiao, Y.; Deng, H.; Yang, H.; He, P.; Zhou, H. Liquid Electrolytes with De-Solvated Lithium Ions for Lithium-Metal Battery. Joule 2020, 4, 1776– 1789,  DOI: 10.1016/j.joule.2020.06.011
      14
      A Liquid Electrolyte with De-Solvated Lithium Ions for Lithium-Metal Battery
      Chang, Zhi; Qiao, Yu; Deng, Han; Yang, Huijun; He, Ping; Zhou, Haoshen
      Joule (2020), 4 (8), 1776-1789CODEN: JOULBR; ISSN:2542-4351. (Cell Press)
      Traditional liq. electrolytes used in rechargeable batteries, fuel cells, and electrochem. capacitors composed of solvents, anions, and solvents solvated cations (e.g., lithium ions, Li+), follow classic ''cations with solvation'' electrolyte configuration and can be defined as ''cations solvated electrolytes.''. In these electrolytes, the de-solvation processes of solvated cations only occur when the cations inserted-deposited on the electrodes' surface. Here, different from traditional electrolytes, a new liq. electrolyte with de-solvated Li+ was discovered (''Li+ de-solvated electrolyte''), since it merely composed of inactive ''frozen-like'' solvent and crystal-like salt solute. Inspiringly, its electrochem. stability was remarkably improved (extended to 4.5 V for ''Li+ de-solvated ether-based electrolyte''). Ultra-stable high-energy-d. lithium-metal batteries (LiNi0.8Co0.1Mn0.1O2//Li) were achieved (half-cell: 140 mAh g-1 after 830 cycles; full-cell: 170 mAh g-1 after 200 cycles under twice excessed Li). It is also surprising that this does not present any cathode-electrolyte interface (CEI) layer on the cycled NCM-811 surface benefit from the ''Li+ de-solvated electrolyte.''.
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    15. 15
      Cavers, H.; Molaiyan, P.; Abdollahifar, M.; Lassi, U.; Kwade, A. Perspectives on Improving the Safety and Sustainability of High Voltage Lithium-Ion Batteries Through the Electrolyte and Separator Region. Adv. Energy Mater. 2022, 12, 2200147,  DOI: 10.1002/aenm.202200147
      15
      Perspectives on Improving the Safety and Sustainability of High Voltage Lithium-Ion Batteries Through the Electrolyte and Separator Region
      Cavers, Heather; Molaiyan, Palanivel; Abdollahifar, Mozaffar; Lassi, Ulla; Kwade, Arno
      Advanced Energy Materials (2022), 12 (23), 2200147CODEN: ADEMBC; ISSN:1614-6840. (Wiley-Blackwell)
      A review. Lithium-ion batteries (LIBs) are promising candidates within the context of the development of novel battery concepts with high energy densities. Batteries with high operating potentials or high voltage (HV) LIBs (>4.2 V vs Li+/Li) can provide high energy densities and are therefore attractive in high-performance LIBs. However, a variety of challenges (including solid electrolyte interface (SEI), lithium plating, etc.) and related safety issues (such as gas formation or thermal runaway effects) must be solved for the practical, widespread application of HV-LIBs. Most of these challenges arise in the region between the electrodes: the electrolyte region. This review provides an overview of recent development and progress on the electrolyte region, including liq. electrolytes, ionic liqs., gel polymer electrolytes, separators, and solid electrolytes for HV-LIBs applications. A focus on improving the safety of these systems, with some perspectives on their relative cost and environmental impact, is given. Overall, the new information is encouraging for the development of HV-LIBs, and this review serves as a guide for potential strategies to improve their safety, allowing the development of HV-LIBs, including solid-state batteries, to be accelerated to practical relevance.
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      Chen, K.-S.; Balla, I.; Luu, N. S.; Hersam, M. C. Emerging Opportunities for Two-Dimensional Materials in Lithium-Ion Batteries. ACS Energy Lett. 2017, 2, 2026– 2034,  DOI: 10.1021/acsenergylett.7b00476
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      Emerging Opportunities for Two-Dimensional Materials in Lithium-Ion Batteries
      Chen, Kan-Sheng; Balla, Itamar; Luu, Norman S.; Hersam, Mark C.
      ACS Energy Letters (2017), 2 (9), 2026-2034CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
      A review. Lithium-ion batteries (LIBs) have achieved widespread utilization as primary rechargeable energy storage devices. In recent years, significant advances have been made in two-dimensional (2D) materials that have the potential to bring unprecedented functionality to next-generation LIBs. While many 2D materials can serve as a new class of active materials that exhibit superlative energy and power densities, they can also be employed as versatile additives that improve the kinetics and stability of LIBs. Here, we present a Perspective on how 2D materials can impact each of the primary components of a LIB including the anode, cathode, conductive additive, electrode-electrolyte interface, separator, and electrolyte. In this manner, emerging opportunities and challenges for 2D materials are identified that can inform future research on high-performance LIBs.
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    17. 17
      Fan, X.; Chen, L.; Borodin, O.; Ji, X.; Chen, J.; Hou, S.; Deng, T.; Zheng, J.; Yang, C.; Liou, S.-C. Non-Flammable Electrolyte Enables Li-Metal Batteries with Aggressive Cathode Chemistries. Nat. Nanotechnol. 2018, 13, 715– 722,  DOI: 10.1038/s41565-018-0183-2
      17
      Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries
      Fan, Xiulin; Chen, Long; Borodin, Oleg; Ji, Xiao; Chen, Ji; Hou, Singyuk; Deng, Tao; Zheng, Jing; Yang, Chongyin; Liou, Sz-Chian; Amine, Khalil; Xu, Kang; Wang, Chunsheng
      Nature Nanotechnology (2018), 13 (8), 715-722CODEN: NNAABX; ISSN:1748-3387. (Nature Research)
      Rechargeable Li-metal batteries using high-voltage cathodes can deliver the highest possible energy densities among all electrochemistries. However, the notorious reactivity of metallic lithium as well as the catalytic nature of high-voltage cathode materials largely prevents their practical application. Here, we report a non-flammable fluorinated electrolyte that supports the most aggressive and high-voltage cathodes in a Li-metal battery. Our battery shows high cycling stability, as evidenced by the efficiencies for Li-metal plating/stripping (99.2%) for a 5 V cathode LiCoPO4 (∼99.81%) and a Ni-rich LiNi0.8Mn0.1Co0.1O2 cathode (∼99.93%). At a loading of 2.0 mAh cm-2, our full cells retain ∼93% of their original capacities after 1,000 cycles. Surface analyses and quantum chem. calcns. show that stabilization of these aggressive chemistries at extreme potentials is due to the formation of a several-nanometer-thick fluorinated interphase.
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    18. 18
      Gond, R.; van Ekeren, W.; Mogensen, R.; Naylor, A. J.; Younesi, R. Non-flammable Liquid Electrolytes for Safe Batteries. Mater. Horiz. 2021, 8, 2913– 2928,  DOI: 10.1039/D1MH00748C
      18
      Non-flammable liquid electrolytes for safe batteries
      Gond, Ritambhara; van Ekeren, Wessel; Mogensen, Ronnie; Naylor, Andrew J.; Younesi, Reza
      Materials Horizons (2021), 8 (11), 2913-2928CODEN: MHAOBM; ISSN:2051-6355. (Royal Society of Chemistry)
      A review. With continual increments in energy d. gradually boosting the performance of rechargeable alkali metal ion . Li+, Na+, K+ batteries, their safe operation is of growing importance and needs to be considered during their development. This is essential, given the high-profile incidents involving battery fires as portrayed by the media. Such hazardous events result from exothermic chem. reactions occurring between the flammable electrolyte and the electrode material under abusive operating conditions. Some classes of non-flammable org. liq. electrolytes have shown potential towards safer batteries with minimal detrimental effect on cycling and, in some cases, even enhanced performance. This article reviews the state-of-the-art in non-flammable liq. electrolytes for Li-, Na- and K-ion batteries. It provides the reader with an overview of carbonate, ether and phosphate-based org. electrolytes, co-solvated electrolytes and electrolytes with flame-retardant additives as well as highly concd. and locally highly concd. electrolytes, ionic liqs. and inorg. electrolytes. Furthermore, the functionality and purpose of the components present in typical non-flammable mixts. are discussed. Moreover, many non-flammable liq. electrolytes are shown to offer improved cycling stability and rate capability compared to conventional flammable liq. electrolytes.
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    19. 19
      Kim, K.; Ma, H.; Park, S.; Choi, N.-S. Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges. ACS Energy Lett. 2020, 5, 1537– 1553,  DOI: 10.1021/acsenergylett.0c00468
      19
      Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges
      Kim, Koeun; Ma, Hyunsoo; Park, Sewon; Choi, Nam-Soon
      ACS Energy Letters (2020), 5 (5), 1537-1553CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
      A review. Electrolyte additives have been explored to attain significant breakthroughs in the long-term cycling performance of lithium-ion batteries (LIBs) without sacrificing energy d.; this has been achieved through the development of stable electrode interfacial structures and the elimination of reactive substances. Here we highlight the potential and the challenges raised by studies on electrolyte additives toward addressing the interfacially induced deterioration of high-capacity electrodes with a focus on Ni-rich layered oxides and Si, which are expected to satisfy the growing demands for high-energy-d. batteries. We also discuss issues with the design of electrolyte additives for practical viability. A deep understanding of the roles of existing electrolyte additives depending on their functional groups will aid in the design of functional additive moieties capable of building robust interfacial layers, scavenging undesired reactive species, and suppressing the gas generation that causes safety hazards and shortened lifetimes of LIBs.
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    20. 20
      Zheng, C. Examining the Benefits of Using Boron Compounds in Lithium Batteries: A Comprehensive Review of Literature. Batteries 2022, 8, 187,  DOI: 10.3390/batteries8100187
      20
      Examining the Benefits of Using Boron Compounds in Lithium Batteries: A Comprehensive Review of Literature
      Zheng, Changlin
      Batteries (Basel, Switzerland) (2022), 8 (10), 187CODEN: BATTAT; ISSN:2313-0105. (MDPI AG)
      A review. Boron and boron compds. have been extensively studied together in the history and development of lithium batteries, which are crucial to decarbonization in the automotive industry and beyond. With a wide examn. of battery components, but a boron-centric approach to raw materials, this review attempts to summarize past and recent studies on the following: which boron compds. are studied in a lithium battery, in which parts of lithium batteries are they studied, what improvements are offered for battery performance, and what improvement mechanisms can be explained. The uniqueness of boron and its extensive application beyond batteries contextualizes the interesting similarity with some studies on batteries. At the end, the article aims to predict prospective trends for future studies that may lead to a more extensive use of boron compds. on a com. scale.
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    21. 21
      Pu, J.; Zhang, K.; Wang, Z.; Li, C.; Zhu, K.; Yao, Y.; Hong, G. Synthesis and Modifications of Boron Nitride Nanomaterials for Electrochemical Energy Storage: From Theory to Application. Adv. Funct. Mater. 2021, 31, 2106315,  DOI: 10.1002/adfm.202106315
      21
      Synthesis and Modification of Boron Nitride Nanomaterials for Electrochemical Energy Storage: From Theory to Application
      Pu, Jun; Zhang, Kai; Wang, Zhenghua; Li, Chaowei; Zhu, Kaiping; Yao, Yagang; Hong, Guo
      Advanced Functional Materials (2021), 31 (48), 2106315CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)
      A review. As a conventional insulating material, boron nitride (BN) has been mainly investigated in the electronics field. Very recently, with the development of prepn./modification technol. and deeper understanding of the electrochem. mechanisms, BN-based nanomaterials have made significant progress in the field of electrochem. Exploiting the characteristics of BN for advanced electrochem. devices is expected to be a breakthrough that will stimulate a new energy revolution. Owing to its chem. and thermal stability, as well as its high mech. strength, BN can alleviate various inherent problems in electrochem. systems, such as thermal deformation of conventional org. separators, weak solid electrolyte interface layers of metal anodes, and electrocatalyst poisoning. The integration of BN with various electrochem. energy technologies is systematically summarized from the perspectives of material prepn., theor. calcns., and practical applications. Moreover, the challenges and prospects for the future development of BN-based electrochem. are highlighted.
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    22. 22
      Rodrigues, M. -T. F.; Kalaga, K.; Gullapalli, H.; Babu, G.; Reddy, A. L. M.; Ajayan, P. M. Hexagonal Boron Nitride-Based Electrolyte Composite for Li-Ion Battery Operation from Room Temperature to 150 °C. Adv. Energy. Mater. 2016, 6, 1600218,  DOI: 10.1002/aenm.201600218
      There is no corresponding record for this reference.
    23. 23
      Molaei, Md. J.; Younas, Md.; Rezakazemi, M. Comprehensive Review on Recent Advances in Two-Dimensional (2D) Hexagonal Boron Nitride. ACS Appl. Electron. Mater. 2021, 3, 5165– 5187,  DOI: 10.1021/acsaelm.1c00720
      23
      A Comprehensive Review on Recent Advances in Two-Dimensional (2D) Hexagonal Boron Nitride
      Molaei, Mohammad Jafar; Younas, Mohammad; Rezakazemi, Mashallah
      ACS Applied Electronic Materials (2021), 3 (12), 5165-5187CODEN: AAEMBP; ISSN:2637-6113. (American Chemical Society)
      A review. Two-dimensional hexagonal boron nitride (2D-hBN) is an emerging 2D material that has received considerable attention due to its exceptional properties including elec. insulation, low dielec. const., easy synthesis, high-temp. stability, corrosion resistance, and chem. stability. 2D-hBN can be integrated with other 2D materials such as graphene in the next-generation of electronic and optoelectronic devices and van der Waals heterostructures. In this review, unique properties of the 2D-hBN are discussed and recent advancements in the synthesis methods such as mech. exfoliation, liq. exfoliation, ion intercalation, chem. vapor deposition, phys. vapor deposition, magnetron sputtering, pulsed laser deposition, ion sputtering deposition, and some more techniques are reviewed. Furthermore, versatile applications of 2D-hBN nanosheets in graphene electronics, tunneling barrier, dielecs., passivation layers, deep UV light sources, single-photon emitters, sensors, and catalysis are critically analyzed. Current challenges and future perspectives for the utilization of 2D-hBN in the next-generation ultrathin electronic devices are discussed.
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    24. 24
      Liu, J.; Cao, D.; Yao, H.; Liu, D.; Zhang, X.; Zhang, Q.; Chen, L.; Wu, S.; Sun, Y.; He, D. Hexagonal Boron Nitride-Coated Polyimide Ion Track Etched Separator with Enhanced Thermal Conductivity and High-Temperature Stability for Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2022, 5, 8639– 8649,  DOI: 10.1021/acsaem.2c01163
      There is no corresponding record for this reference.
    25. 25
      Rahman, M. M.; Mateti, S.; Cai, Q.; Sultana, I.; Fan, Y.; Wang, X.; Hou, C.; Chen, Y. High Temperature and High-Rate Lithium-Ion Batteries with Boron Nitride Nanotubes Coated Polypropylene Separators. Energy Storage Mater. 2019, 19, 352– 359,  DOI: 10.1016/j.ensm.2019.03.027
      There is no corresponding record for this reference.
    26. 26
      Jakubinek, M. B.; Kim, K. S.; Kim, M. J.; Martí, A. A.; Pasquali, M. Recent Advances and Perspective on Boron Nitride Nanotubes: From Synthesis to Applications. J. Mater. Res. 2022, 37, 4403– 4418,  DOI: 10.1557/s43578-022-00841-6
      26
      Recent advances and perspective on boron nitride nanotubes: From synthesis to applications
      Jakubinek, Michael B.; Kim, Keun Su; Kim, Myung Jong; Marti, Angel A.; Pasquali, Matteo
      Journal of Materials Research (2022), 37 (24), 4403-4418CODEN: JMREEE; ISSN:2044-5326. (Springer International Publishing AG)
      A review. Boron nitride nanotubes (BNNTs) are emerging nanomaterials with analogous structures and similarly impressive mech. properties to carbon nanotubes (CNTs), but unique chem. and complimentary multifunctional properties, including higher thermal stability, elec. insulation, optical transparency, neutron absorption capability, and piezoelectricity. Over the past decade, advances in synthesis have made BNNTs more broadly accessible to the nanomaterials and other research communities, removing a major barrier to their utilization and research. Therefore, the field is poised to grow rapidly and see the emergence of BNNT applications ranging from electronics to aerospace materials. A key challenge, that is being gradually overcome, is the development of manufg. processes to make "neat" BNNT materials. This overview highlights the history and current status of the field, providing both an introduction to this Focus Issue-BNNTs: Synthesis to Applications-as well as a perspective on advances, challenges, and opportunities for this emerging material.
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    27. 27
      Chava, B. D.; Wang, Y.; Das, S. Boron Nitride Nanotube–Salt–Water Hybrid: Toward Zero-Dimensional Liquid Water and Highly Trapped Immobile Single Anions Inside One-Dimensional Nanostructures. J. Phys. Chem. C 2021, 125, 14006– 14013,  DOI: 10.1021/acs.jpcc.1c01683
      27
      Boron Nitride Nanotube-Salt-Water Hybrid: Toward Zero-Dimensional Liquid Water and Highly Trapped Immobile Single Anions Inside One-Dimensional Nanostructures
      Chava, Bhargav Sai; Wang, Yanbin; Das, Siddhartha
      Journal of Physical Chemistry C (2021), 125 (25), 14006-14013CODEN: JPCCCK; ISSN:1932-7447. (American Chemical Society)
      Nanotube-mol.-based hybrid structures, where different chem. species are integrated with the nanotubes either exohedrally (i.e., attached on the outer surface of the nanotubes) or endohedrally (i.e., encapsulated within the nanotubes), have enabled developing novel materials with unprecedented application potential. In this paper, we describe our simulation-driven discovery of an endohedral and noncovalent nanotube-salt-water [boron nitride nanotube (BNNT)-LiTFSI-water] hybrid structure, which forms when a 1 nm diam. BNNT, placed in a large-concn. LiTFSI electrolyte soln., gets filled with periodically repeating and axially sepd. nonoverlapping blocks of the TFSI anion and Li-ion-solvating water. In this hybrid structure, the TFSI anions are in highly trapped immobile state, while the water blocks are in a zero-dimensional configuration and a liq. (noncryst.) state. Furthermore, subjecting the hybrid to elevated temp. or salt-free surrounding has little effect on the structure and properties of this hybrid. This, along with sep. free energy simulations, confirms the most remarkable stability of this nanotube-salt-water hybrid system.
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    28. 28
      Kim, J.; Seo, D.; Yoo, J.; Jeong, W.; Seo, Y.-S.; Kim, J. High Purity and Yield of Boron Nitride Nanotubes Using Amorphous Boron and a Nozzle-Type Reactor. Materials 2014, 7, 5789– 5801,  DOI: 10.3390/ma7085789
      28
      High purity and yield of boron nitride nanotubes using amorphous boron and a nozzle-type reactor
      Kim, Jaewoo; Seo, Duckbong; Yoo, Jeseung; Jeong, Wanseop; Seo, Young-Soo; Kim, Jaeyong
      Materials (2014), 7 (8), 5789-5801CODEN: MATEG9; ISSN:1996-1944. (MDPI AG)
      Enhancement of the prodn. yield of boron nitride nanotubes (BNNTs) with high purity was achieved using an amorphous boron-based precursor and a nozzle-type reactor. Use of a mixt. of amorphous boron and Fe decreases the milling time for the prepn. of the precursor for BNNTs synthesis, as well as the Fe impurity contained in the B/Fe interdiffused precursor nanoparticles by using a simple purifn. process. We also explored a nozzle-type reactor that increased the prodn. yield of BNNTs compared to a conventional flow-through reactor. By using a nozzle-type reactor with amorphous boron-based precursor, the wt. of the BNNTs sample after annealing was increased as much as 2.5-times with much less impurities compared to the case for the flow-through reactor with the cryst. boron-based precursor. Under the same exptl. conditions, the yield and quantity of BNNTs were estd. as much as ∼70% and ∼1.15 g/batch for the former, while they are ∼54% and 0.78 g/batch for the latter.
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    29. 29
      Kim, J.; Lee, S.; Uhm, Y. R.; Jun, J.; Rhee, C. K.; Kim, G. M. Synthesis and Growth of Boron Nitride Nanotubes by a Ball Milling–Annealing Process. Acta Mater. 2011, 59, 2807– 2813,  DOI: 10.1016/j.actamat.2011.01.019
      29
      Synthesis and growth of boron nitride nanotubes by a ball milling-annealing process
      Kim, Jaewoo; Lee, Sol; Uhm, Young Rang; Jun, Jiheon; Rhee, Chang Kyu; Kim, Gil Moo
      Acta Materialia (2011), 59 (7), 2807-2813CODEN: ACMAFD; ISSN:1359-6454. (Elsevier Ltd.)
      The synthesis and growth of boron nitride nanotubes (BNNTs) based on ball milling of cryst. boron powder followed by heat treatment were investigated. Fe-based stainless steel (STS) balls and milling vessels were used for milling, and the Fe impurity produced during milling acts as a catalyst for the generation of BNNTs during annealing under a nitrogen environment. Structural deformation of cryst. boron was obsd. for milled boron powder based on X-ray diffraction spectra and electron microscopy images. No chem. reactions of boron with nitrogen occurred during milling, and BNNTs were only synthesized during annealing. The BNNTs produced are basically multi-walled cylindrical- or bamboo-types mixed into nanotube clusters. The diams. of BNNTs are in the range of 50-150 nm, and nos. of the walls are 30-100 with a ∼0.3 nm gap on av. It was obsd. that BN was synthesized from amorphous boron coated onto the surface of the Fe particles. In addn., the types of grown nanotubes could be detd. by the initial shapes of BN clusters on a Fe catalyst particle, which are nanoshells or opened nanocylinders. Yields of BNNTs were strongly dependent on the amorphous structure of the boron particles rather than on the residual cryst. boron particles in the milled samples.
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    30. 30
      Zhang, F.; Nemeth, K.; Bareno, J.; Dogan, F.; Bloom, I. D.; Shaw, L. L. Experimental and Theoretical Investigations of Functionalized Boron Nitride as Electrode Materials for Li-ion Batteries. RSC Adv. 2016, 6, 27901– 27914,  DOI: 10.1039/C6RA03141B
      30
      Experimental and theoretical investigations of functionalized boron nitride as electrode materials for Li-ion batteries
      Zhang, Fan; Nemeth, Karoly; Bareno, Javier; Dogan, Fulya; Bloom, Ira D.; Shaw, Leon L.
      RSC Advances (2016), 6 (33), 27901-27914CODEN: RSCACL; ISSN:2046-2069. (Royal Society of Chemistry)
      The feasibility of synthesizing functionalized h-BN (FBN) via the reaction between molten LiOH and solid h-BN is studied for the first time and its first ever application as an electrode material in Li-ion batteries is evaluated. D. functional theory (DFT) calcns. are performed to provide mechanistic understanding of the possible electrochem. reactions derived from the FBN. Various materials characterizations reveal that the melt-solid reaction can lead to exfoliation and functionalization of h-BN simultaneously, while electrochem. anal. proves that the FBN can reversibly store charges through surface redox reactions with good cycle stability and coulombic efficiency. DFT calcns. have provided phys. insights into the obsd. electrochem. properties derived from the FBN.
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    31. 31
      Pfaffenhuber, C.; Maier, J. Quantitative estimate of the conductivity of a soggy sand electrolyte: example of (LiClO4, THF):SiO2. J. Phys. Chem. Chem. Phys. 2013, 15, 2050– 2054,  DOI: 10.1039/C2CP43561F
      There is no corresponding record for this reference.
    32. 32
      Hofmann, A.; Migeot, M.; Thißen, E.; Schulz, M.; Heinzmann, R.; Indris, S.; Bergfeldt, T.; Lei, B.; Ziebert, C.; Hanemann, T. Electrolyte Mixtures Based on Ethylene Carbonate and Dimethyl Sulfone for Li-Ion Batteries with Improved Safety Characteristics. ChemSusChem 2015, 8, 1892– 1900,  DOI: 10.1002/cssc.201500263
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      Electrolyte Mixtures Based on Ethylene Carbonate and Dimethyl Sulfone for Li-Ion Batteries with Improved Safety Characteristics
      Hofmann, Andreas; Migeot, Matthias; Thissen, Eva; Schulz, Michael; Heinzmann, Ralf; Indris, Sylvio; Bergfeldt, Thomas; Lei, Boxia; Ziebert, Carlos; Hanemann, Thomas
      ChemSusChem (2015), 8 (11), 1892-1900CODEN: CHEMIZ; ISSN:1864-5631. (Wiley-VCH Verlag GmbH & Co. KGaA)
      In this study, novel electrolyte mixts. for Li-ion cells are presented with highly improved safety features. The electrolyte formulations are composed of ethylene carbonate/dimethyl sulfone (80:20 wt/wt) as the solvent mixt. and LiBF4, lithium bis(trifluoromethanesulfonyl)azanide, and lithium bis(oxalato)borate as the conducting salts. Initially, the electrolytes are characterized with regard to their phys. properties, their lithium transport properties, and their electrochem. stability. The key advantages of the electrolytes are high flash points of >140 °C, which enhance significantly the intrinsic safety of Li-ion cells contg. these electrolytes. This has been quantified by measurements in an accelerating rate calorimeter. By using the newly developed electrolytes, which are liq. down to T=-10 °C, it is possible to achieve C-rates of up to 1.5 C with >80 % of the initial specific capacity. During 100 cycles in cell tests (graphite||LiNi1/3Co1/3Mn1/3O2), it is proven that the retention of the specific capacity is >98 % of the third discharge cycle with dependence on the conducting salt. The best electrolyte mixt. yields a capacity retention of >96 % after 200 cycles in coin cells.
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    33. 33
      Sun, Z.; Li, F.; Ding, J.; Lin, Z.; Xu, M.; Zhu, M.; Liu, J. High-Voltage and High-Temperature LiCoO2 Operation via the Electrolyte Additive of Electron-Defect Boron Compounds. ACS Energy Lett. 2023, 8, 2478– 2487,  DOI: 10.1021/acsenergylett.3c00324
      33
      High-Voltage and High-Temperature LiCoO2 Operation via the Electrolyte Additive of Electron-Defect Boron Compounds
      Sun, Zhaoyu; Li, Fangkun; Ding, Jieying; Lin, Zhiye; Xu, Mengqing; Zhu, Min; Liu, Jun
      ACS Energy Letters (2023), 8 (6), 2478-2487CODEN: AELCCP; ISSN:2380-8195. (American Chemical Society)
      Com. LIBs have the problem of instability interface of electrolyte/cathode at high voltage and high temp. This work reports a novel series of electron-defect boron compds. to construct stable interfaces of LCO/electrolyte. The results of theor. calcn. indicate that compds. of DPD scaffold can win in the competitive oxidn. decompn. for interface regulation. F-rich and B-rich interface is designed by modifying the functional group of DPD scaffold. This strategy of in situ interface design successfully suppresses the dissoln. of harmful transition metal ions and the nucleophilic reaction between electrolyte and cathode. Li/LCO cell can remain stable at high voltage (4.5 V) and high temp. (70 °C) in com. carbonate electrolyte after DPD-F interphase formation. Meanwhile, faster Li+ extn. and insertion kinetics of DPD-F-interface make the Li/LCO cell stable at 4.6 V. Spectral characterizations and theor. calcns. uncover the secret of the forming process of this DPD-F-interface.
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    34. 34
      Li, Q.; Jiao, S.; Luo, L.; Ding, M. S.; Zheng, J.; Cartmell, S. S.; Wang, C.-M.; Xu, K.; Zhang, J.-G.; Xu, W. Wide-Temperature Electrolytes for Lithium-Ion Batteries. ACS Appl. Mater. Interfaces 2017, 9, 18826– 18835,  DOI: 10.1021/acsami.7b04099
      34
      Wide-Temperature Electrolytes for Lithium-Ion Batteries
      Li, Qiuyan; Jiao, Shuhong; Luo, Langli; Ding, Michael S.; Zheng, Jianming; Cartmell, Samuel S.; Wang, Chong-Min; Xu, Kang; Zhang, Ji-Guang; Xu, Wu
      ACS Applied Materials & Interfaces (2017), 9 (22), 18826-18835CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
      Formulating electrolytes with solvents of low f.ps. and high dielec. consts. is a direct approach to extend the service-temp. range of lithium (Li)-ion batteries (LIBs). In this study, we report such wide-temp. electrolyte formulations by optimizing the ethylene carbonate (EC) content in the ternary solvent system of EC, propylene carbonate (PC), and Et Me carbonate (EMC) with LiPF6 salt and CsPF6 additive. An extended service-temp. range from -40 to 60 °C was obtained in LIBs with lithium nickel cobalt aluminum oxide (LiNi0.80Co0.15Al0.05O2, NCA) as cathode and graphite as anode. The discharge capacities at low temps. and the cycle life at room temp. and elevated temps. were systematically investigated together with the ionic cond. and phase-transition behaviors. The most promising electrolyte formulation was identified as 1.0 M LiPF6 in EC-PC-EMC (1:1:8 by wt) with 0.05 M CsPF6, which was demonstrated in both coin cells of graphite‖NCA and 1 Ah pouch cells of graphite‖LiNi1/3Mn1/3Co1/3O2. This optimized electrolyte enables excellent wide-temp. performances, as evidenced by the high capacity retention (68%) at -40 °C and C/5 rate, significantly higher than that (20%) of the conventional LIB electrolyte, and the nearly identical stable cycle life as the conventional LIB electrolyte at room temp. and elevated temps. up to 60 °C.
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    35. 35
      Silva, W. M.; Ribeiro, H.; Taha-Tijerina, J. J. Potential Production of Theranostic Boron Nitride Nanotubes (64Cu-BNNTs) Radiolabeled by Neutron Capture. Nanomaterials 2021, 11, 2907,  DOI: 10.3390/nano11112907
      35
      Potential Production of Theranostic Boron Nitride Nanotubes (64Cu-BNNTs) Radiolabeled by Neutron Capture
      Silva, Wellington Marcos; Ribeiro, Helio; Taha-Tijerina, Jose Jaime
      Nanomaterials (2021), 11 (11), 2907CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
      In this work, the radioisotope 64Cu was obtained from copper (II) chloride dihydrate in a nuclear research reactor by neutron capture, (63Cu(n, γ)64Cu), and incorporated into boron nitride nanotubes (BNNTs) using a solvothermal process. The produced 64Cu-BNNTs were analyzed by TEM, MEV, FTIR, XDR, XPS and gamma spectrometry, with which it was possible to observe the formation of 64Cu nanoparticles, with sizes of up to 16 nm, distributed through nanotubes. The synthesized of 64Cu nanostructures showed a pure photoemission peak of 511 keV, which is characteristic of gamma radiation. This type of emission is desirable for photon emission tomog. (PET scan) image acquisition, as well as its use in several cancer treatments. Thus, 64Cu-BNNTs present an excellent alternative as theranostic nanomaterials that can be used in diagnosis and therapy by different techniques used in nuclear medicine.
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    36. 36
      Dietrich, P. M.; Gehrlein, J.; Maibach, j.; Thissen, A. Probing Lithium-Ion Battery Electrolytes with Laboratory Near-Ambient Pressure XPS. Crystals 2020, 10, 1056,  DOI: 10.3390/cryst10111056
      36
      Probing lithium-ion battery electrolytes with laboratory near-ambient pressure XPS
      Dietrich, Paul M.; Gehrlein, Lydia; Maibach, Julia; Thissen, Andreas
      Crystals (2020), 10 (11), 1056CODEN: CRYSBC; ISSN:2073-4352. (MDPI AG)
      In this article, we present Near Ambient Pressure (NAP)-XPS results from model and com. liq. electrolytes for lithium-ion battery prodn. using an automated lab. NAP-XPS system. The electrolyte solns. were (i) LiPF6 in EC/DMC (LP30) as a typical com. battery electrolyte and (ii) LiTFSI in PC as a model electrolyte. We analyzed the LP30 electrolyte soln., first in its vapor and liq. phase to compare individual core-level spectra. In a second step, we immersed a V2O5 crystal as a model cathode material in this LiPF6 soln. Addnl., the LiTFSI electrolyte model system was studied to compare and verify our findings with previous NAP-XPS data. Photoelectron spectra recorded at pressures of 2-10 mbar show significant chem. differences for the different lithium-based electrolytes. We show the enormous potential of lab. NAP-XPS instruments for investigations of solid-liq. interfaces in electrochem. energy storage systems at elevated pressures and illustrate the simplicity and ease of the used exptl. setup (EnviroESCA).
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    37. 37
      Matsoso, J. B.; Vuillet-a-Ciles, V.; Bois, L.; Toury, B.; Journet, C. Improving Formation Conditions and Properties of hBN Nanosheets Through BaF2-assisted Polymer Derived Ceramics (PDCs) Technique. Nanomaterials 2020, 10, 443,  DOI: 10.3390/nano10030443
      37
      Improving formation conditions and properties of hBN nanosheets through BaF2-assisted polymer derived ceramics (PDCs) technique
      Matsoso, Boitumelo J.; Vuillet-a-Ciles, Victor; Bois, Laurence; Toury, Berangere; Journet, Catherine
      Nanomaterials (2020), 10 (3), 443CODEN: NANOKO; ISSN:2079-4991. (MDPI AG)
      Hexagonal boron nitrite (hBN) is an attractive material for many applications such as in electronics as a complement to graphene, in anti-oxidn. coatings, light emitters, etc. However, the synthesis of high-quality hBN at cost-effective conditions is still a great challenge. Thus, this work reports on the synthesis of large-area and cryst. hBN nanosheets via the modified polymer derived ceramics (PDCs) process. The addn. of both the BaF2 and Li3N, as melting-point redn. and crystn. agents, resp., led to the prodn. of hBN powders with excellent physicochem. properties at relatively low temps. and atm. pressure conditions. For instance, XRD, Raman, and XPS data revealed improved crystallinity and quality at a decreased formation temp. of 1200°C upon the addn. of 5 wt% of BaF2. Moreover, morphol. detn. illustrated the formation of multi-layered nanocryst. and well-defined shaped hBN powders with crystal sizes of 2.74-8.41 ± 0.71μm in diam. Despite the compromised thermal stability, as shown by the ease of oxidn. at high temps., this work paves way for the prodn. of large-scale and high-quality hBN crystals at a relatively low temp. and atm. pressure conditions.
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    38. 38
      Charles-Blin, Y.; Nemoto, K.; Zettsu, N.; Teshima, K. Effects of a Solid Electrolyte Coating on the Discharge Kinetics of a LiCoO2 Electrode: Mechanism and Potential Applications. J. Mater. Chem. A 2020, 8, 20979– 20986,  DOI: 10.1039/D0TA05656A
      38
      Effects of a solid electrolyte coating on the discharge kinetics of a LiCoO2 electrode: mechanism and potential applications
      Charles-Blin, Youn; Nemoto, Kazune; Zettsu, Nobuyuki; Teshima, Katsuya
      Journal of Materials Chemistry A: Materials for Energy and Sustainability (2020), 8 (40), 20979-20986CODEN: JMCAET; ISSN:2050-7496. (Royal Society of Chemistry)
      The application of a Li+-conductive amorphous Li2B4O7 coating on a LiCoO2 electrode enhanced its discharge kinetics by increasing the local concn. of Li+ at the surface of LiCoO2 particles. The origin of internal resistance in Li+ intercalation steps was elucidated by electrochem. impedance spectroscopy (EIS)-based characterization of discharge kinetics for states of charges of 0, 50, and 100%, while the activation energies of intercalation steps were detd. from EIS data collected at different temps. (-10, 0, 20, and 40°C). The activation energy of Li+ desolvation was smaller than that previously reported for bare LiCoO2 particles, which suggested that the significant changes in kinetics assocd. with polarization mitigation were due to the Li+ exchange reaction (Li+ adsorption and diffusion processes) on the surface of LiCoO2 particles. Finally, C-rate capability tests performed at -10°C revealed that the capacity retention of the electrode comprising Li2B4O7-coated LiCoO2 particles exceeded that of the electrode comprising bare LiCoO2 particles (45% vs. 18%, resp.).
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    39. 39
      Zhang, D.; Zhang, S.; Yapici, N.; Oakley, R.; Sharma, S.; Parashar, V.; Yap, Y. K. Emerging Applications of Boron Nitride Nanotubes in Energy Harvesting, Electronics, and Biomedicine. ACS Omega 2021, 6, 20722– 20728,  DOI: 10.1021/acsomega.1c02586
      39
      Emerging Applications of Boron Nitride Nanotubes in Energy Harvesting, Electronics, and Biomedicine
      Zhang, Dongyan; Zhang, Siqi; Yapici, Nazmiye; Oakley, Rodney; Sharma, Sambhawana; Parashar, Vyom; Yap, Yoke Khin
      ACS Omega (2021), 6 (32), 20722-20728CODEN: ACSODF; ISSN:2470-1343. (American Chemical Society)
      A review. Boron nitride nanotubes (BNNTs) are structurally and mech. similar to carbon nanotubes (CNTs). In contrast, BNNTs exhibit unique properties for being elec. insulating and optically transparent due to the polarized boron nitride bonds. All these properties have prevented the use of BNNTs for energy harvesting and electronic devices for more than 25 years. During the past few years, researchers have started to demonstrate a series of novel applications of BNNTs based on unique properties not found on CNTs. For example, these novel applications include osmotic power harvesting using the charged inner surfaces of BNNTs, room-temp. single-electron transistors using insulating BNNTs as the tunneling channels, high-brightness fluorophores that can be 1000-times brighter than regular dyes, and transistors based on Tellurium at. chains filled inside BNNTs. We have reviewed some of these emerging applications and provided our perspective for future work.
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    40. 40
      Cheng, X.-B.; Zhang, R.; Zhao, C.-Z.; Zhang, Q. Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review. Chem. Rev. 2017, 117, 10403– 10473,  DOI: 10.1021/acs.chemrev.7b00115
      40
      Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review
      Cheng, Xin-Bing; Zhang, Rui; Zhao, Chen-Zi; Zhang, Qiang
      Chemical Reviews (Washington, DC, United States) (2017), 117 (15), 10403-10473CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)
      A review is presented. The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-d. energy storage devices in our modern and technol.-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and tech. challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quant. models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theor. understanding and anal., recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applications is included. A general conclusion and a perspective on the current limitations and recommended future research directions of lithium metal batteries are presented. The review concludes with an attempt at summarizing the theor. and exptl. achievements in lithium metal anodes and endeavors to realize the practical applications of lithium metal batteries.
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    41. 41
      Choi, K.-I.; Yadav, D.; Jung, J.; Park, E.; Lee, K.-M.; Kim, T.; Kim, J. Noble Metal Nanoparticles Decorated Boron Nitride Nanotubes for Efficient and Selective Low-Temperature Catalytic Reduction of Nitric Oxide with Carbon Monoxide. ACS Appl. Mater. Interfaces 2023, 15, 10670– 10678,  DOI: 10.1021/acsami.2c20985
      41
      Noble Metal Nanoparticles Decorated Boron Nitride Nanotubes for Efficient and Selective Low-Temperature Catalytic Reduction of Nitric Oxide with Carbon Monoxide
      Choi, Ki-In; Yadav, Dolly; Jung, Junghwan; Park, Eunkwang; Lee, Kyung-Min; Kim, Taejin; Kim, Jaewoo
      ACS Applied Materials & Interfaces (2023), 15 (8), 10670-10678CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)
      Parallel to CO2 emission, NOx emission has become one of the menacing problems that seek a simple, durable, and high-efficiency deNOx catalyst. Herein, the authors demonstrated simple syntheses of Pt group metal nanoparticle-decorated f-BNNT (PGM = Pd, Pt, and Rh, and f-BNNT stands for -OH-functionalized B nitride nanotubes) as a catalyst for efficient and selective redn. of NO by CO at low-temp. conditions. PGM/f-BNNT with a low amt. of noble metal nanoparticles (0.7-0.8%) presents very efficient catalytic activity for NO redn. as well as CO oxidn. during their removal process. The removal efficiencies of NO and CO with Pd/f-BNNT, Pt/f-BNNT, and Rh/f-BNNT catalysts were studied under various temps., flow rates, and reaction times, resp. For most cases, NO catalytic redn. with CO reaction was >99% at a temp. as low as ~ 200°. The catalyst robustness and efficiency were also verified by presenting almost 100% conversion of NO using a Rh/f-BNNT catalyst, which was aged under humid air at 600 and 700° for 24 h, resp. The synergic effect of the catalytic efficacy of the well-dispersed noble metal nanoparticles and the excellent surface properties of BNNT are reasons for the high selectivity and catalytic property at a low temp. The noble metal nanoparticle-decorated f-BNNT catalysts are possible to save expensive PGM catalysts, such as Pt, Pd, and Rd, ≤100 times while presenting similar or better catalytic performance for simultaneous NO and CO removals.
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    42. 42
      Li, Y.; Zhang, L.; Sun, Z.; Gao, G.; Lu, S.; Zhu, M.; Zhang, Y.; Jia, Z.; Xiao, C.; Bu, H.; Xi, K.; Ding, S. Hexagonal Boron Nitride Induces Anion Trapping in a Polyethylene Oxide Based Solid Polymer Electrolyte for Lithium Dendrite Inhibition. J. Mater. Chem. A 2020, 8, 9579– 9589,  DOI: 10.1039/D0TA03677C
      42
      Hexagonal boron nitride induces anion trapping in a polyethylene oxide based solid polymer electrolyte for lithium dendrite inhibition
      Li, Yuhan; Zhang, Libo; Sun, Zongjie; Gao, Guoxin; Lu, Shiyao; Zhu, Min; Zhang, Yanfeng; Jia, Zhiyu; Xiao, Chunhui; Bu, Huaitian; Xi, Kai; Ding, Shujiang
      Journal of Materials Chemistry A: Materials for Energy and Sustainability (2020), 8 (19), 9579-9589CODEN: JMCAET; ISSN:2050-7496. (Royal Society of Chemistry)
      Here a hexagonal boron nitride (h-BN)-polyethylene oxide composite polymer electrolyte is prepd. via a convenient casting method, which shows high mech. strength. Meanwhile, the electrochem. properties (electrochem. window and lithium ion transference no.) are enhanced but the ionic cond. of the h-BN composite electrolyte is decreased after adding h-BN. D. functional theory (DFT) calcn. results show that a stronger binding effect is obsd. between TFSI- and BN, compared to that between Li+ and BN. Mol. dynamics (MD) simulations are also utilized to study the mechanism behind the enhanced Li ion diffusion by h-BN addn. Li+ diffusion in PEO/LiTFSI/BN is lower than that in the PEO/LiTFSI system, but the diffusion of TFSI- exhibits a more significant decline rate in the presence of BN. This indicates that the presence of BN suppresses anion motion and enhances selectivity in Li+ transport. Thus, the PEO/LiTFSI/h-BN composite electrolyte exhibits higher Li ion cond. but lower anion diffusivity than the PEO/LiTFSI system. Hence the h-BN composite polymer electrolyte in a Li/Li sym. battery provides a long cycling time of 430 h at 0.2 mA cm-2. A Li metal/LiFePO4 full battery with the PEO/LiTFSI/h-BN composite electrolyte also works more efficiently for long-term cycling (140 cycles) than a filler-free PEO based electrolyte (39 cycles).
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    43. 43
      Cetindag, S.; Tiwari, B.; Zhang, D.; Yap, Y. K.; Kim, S.; Shan, J. Surface-Charge Effects on the Electro-Orientation of Insulating Boron-Nitride Nanotubes in Aqueous Suspension. J. Colloid Interface Sci. 2017, 505, 1185– 1192,  DOI: 10.1016/j.jcis.2017.05.073
      43
      Surface-charge effects on the electro-orientation of insulating boron-nitride nanotubes in aqueous suspension
      Cetindag, Semih; Tiwari, Bishnu; Zhang, Dongyan; Yap, Yoke Khin; Kim, Sangil; Shan, Jerry W.
      Journal of Colloid and Interface Science (2017), 505 (), 1185-1192CODEN: JCISA5; ISSN:0021-9797. (Elsevier B.V.)
      The alignment of hexagonal boron-nitride nanotubes (BNNTs) in aq. KCl solns. under spatially uniform elec. fields was examd. exptl., using direct optical visualization to probe the orientation dynamics of individual BNNTs for different elec.-field frequencies. Different from most previously studied nanowires and nanotubes, BNNTs are wide-bandgap materials which are essentially insulating at room temp. The authors analyze the electro-orientation of BNNTs in the general context of polarizable cylindrical particles in liq. suspensions, whose behavior can fall into different regimes, including alignment due to Maxwell-Wagner induced dipoles at high frequencies, and alignment due to fluid motion of the elec. double layer around the particles at lower frequencies. For BNNTs, the variation of the crossover frequencies in the electro-orientation spectra was studied in electrolytes of different cond. The effect of BNNT surface charge on electro-orientation was further studied by changing the pH of the aq. soln. The authors find that the elec.-field alignment of the BNNTs in the low-frequency regime is assocd. with the charging and motion of the elec. double layer around the particle. However, as BNNTs are non-conducting particles, the reasons for the formation of the elec. double layer are likely to be different than that of conducting particles. The authors discuss two possible mechanisms for the double-layer formation and alignment of 1D dielec. particles, and make comparison to those for the more commonly studied conducting particles.
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    44. 44
      Zuo, K.; Zhang, X.; Huang, X.; Oliveira, E. F.; Guo, H.; Zhai, T.; Wang, W.; Alvarez, P. J. J.; Elimelech, M.; Ajayan, P. K.; Lou, J.; Li, Q. Ultrahigh Resistance of Hexagonal Boron Nitride to Mineral Scale Formation. Nat. Commun. 2022, 13, 4523,  DOI: 10.1038/s41467-022-32193-4
      44
      Ultrahigh resistance of hexagonal boron nitride to mineral scale formation
      Zuo, Kuichang; Zhang, Xiang; Huang, Xiaochuan; Oliveira, Eliezer F.; Guo, Hua; Zhai, Tianshu; Wang, Weipeng; Alvarez, Pedro J. J.; Elimelech, Menachem; Ajayan, Pulickel M.; Lou, Jun; Li, Qilin
      Nature Communications (2022), 13 (1), 4523CODEN: NCAOBW; ISSN:2041-1723. (Nature Portfolio)
      Abstr.: Formation of mineral scale on a material surface has profound impact on a wide range of natural processes as well as industrial applications. However, how specific material surface characteristics affect the mineral-surface interactions and subsequent mineral scale formation is not well understood. Here we report the superior resistance of hexagonal boron nitride (hBN) to mineral scale formation compared to not only common metal and polymer surfaces but also the highly scaling-resistant graphene, making hBN possibly the most scaling resistant material reported to date. Exptl. and simulation results reveal that this ultrahigh scaling-resistance is attributed to the combination of hBNs atomically-smooth surface, in-plane at. energy corrugation due to the polar boron-nitrogen bond, and the close match between its interat. spacing and the size of water mols. The latter two properties lead to strong polar interactions with water and hence the formation of a dense hydration layer, which strongly hinders the approach of mineral ions and crystals, decreasing both surface heterogeneous nucleation and crystal attachment.
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    45. 45
      Siria, A.; Poncharal, P.; Biance, A. L.; Fulcrand, R.; Blasé, X.; Purcell, S. T.; Bocquet, L. Giant Osmotic Energy Conversion Measured in a Single Transmembrane Boron Nitride Nanotube. Nature 2013, 494, 455– 458,  DOI: 10.1038/nature11876
      45
      Giant osmotic energy conversion measured in a single transmembrane boron nitride nanotube
      Siria, Alessandro; Poncharal, Philippe; Biance, Anne-Laure; Fulcrand, Remy; Blase, Xavier; Purcell, Stephen T.; Bocquet, Lyderic
      Nature (London, United Kingdom) (2013), 494 (7438), 455-458CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
      New models of fluid transport are expected to emerge from the confinement of liqs. at the nanoscale, with potential applications in ultrafiltration, desalination and energy conversion. Nevertheless, advancing our fundamental understanding of fluid transport on the smallest scales requires mass and ion dynamics to be ultimately characterized across an individual channel to avoid averaging over many pores. A major challenge for nanofluidics thus lies in building distinct and well-controlled nanochannels, amenable to the systematic exploration of their properties. Here we describe the fabrication and use of a hierarchical nanofluidic device made of a boron nitride nanotube that pierces an ultrathin membrane and connects two fluid reservoirs. Such a transmembrane geometry allows the detailed study of fluidic transport through a single nanotube under diverse forces, including elec. fields, pressure drops and chem. gradients. Using this device, we discover very large, osmotically induced elec. currents generated by salinity gradients, exceeding by two orders of magnitude their pressure-driven counterpart. We show that this result originates in the anomalously high surface charge carried by the nanotube's internal surface in water at large pH, which we independently quantify in conductance measurements. The nano-assembly route using nanostructures as building blocks opens the way to studying fluid, ionic and mol. transport on the nanoscale, and may lead to biomimetic functionalities. Our results furthermore suggest that boron nitride nanotubes could be used as membranes for osmotic power harvesting under salinity gradients.
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    46. 46
      Kim, D.; Liu, X.; Yu, B.; Mateti, S.; O’Dell, L. A.; Rong, Q.; Chen, Y. Amine-Functionalized Boron Nitride Nanosheets: A New Functional Additive for Robust, Flexible Ion Gel Electrolyte with High Lithium-Ion Transference Number. Adv. Funct. Mater. 2020, 30, 1910813,  DOI: 10.1002/adfm.201910813
      46
      Amine-Functionalized Boron Nitride Nanosheets: A New Functional Additive for Robust, Flexible Ion Gel Electrolyte with High Lithium-Ion Transference Number
      Kim, Donggun; Liu, Xin; Yu, Baozhi; Mateti, Srikanth; O'Dell, Luke A.; Rong, Qiangzhou; Chen, Ying
      Advanced Functional Materials (2020), 30 (15), 1910813CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)
      Ion gel electrolytes show great potential in solid-state batteries attributed to their outstanding characteristics. However, because of the strong ionic nature of ionic liqs., ion gel electrolytes generally exhibit low lithium-ion transference no., limiting its practical application. Amine-functionalized boron nitride (BN) nanosheets (AFBNNSs) are used as an additive into ion gel electrolytes for improving their ion transport properties. The AFBNNSs-ion gel shows much improved mech. strength and thermal stability. The lithium-ion transference no. is increased from 0.12-0.23 due to AFBNNS addn. More importantly, for the first time, NMR anal. reveals that the amine groups on the BN nanosheets have strong interaction with the bis(trifluoromethanesulfonyl)imide anions, which significantly reduces the anion mobility and consequently increases lithium-ion mobility. Battery cells using the optimized AFBNNSs-ion gel electrolyte exhibit stable lithium deposition and excellent electrochem. performance. A LiFePO4|Li cell retains 92.2% of its initial specific capacity after the 60th cycle while the cell without AFBNNSs-gel electrolyte only retains 53.5%. The results not only demonstrate a new strategy to improve lithium-ion transference no. in ionic liq. electrolytes, but also open up a potential avenue to achieve solid-state lithium metal batteries with improved performance.
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    47. 47
      Liu, W.; Lee, S. W.; Lin, D.; Shi, F.; Wang, S.; Sendek, A. D.; Cui, Y. Enhancing Ionic Conductivity in Composite Polymer Electrolytes with Well-Aligned Ceramic Nanowires. Nat. Energy 2017, 2, 17035,  DOI: 10.1038/nenergy.2017.35
      47
      Enhancing ionic conductivity in composite polymer electrolytes with well-aligned ceramic nanowires
      Liu, Wei; Lee, Seok Woo; Lin, Dingchang; Shi, Feifei; Wang, Shuang; Sendek, Austin D.; Cui, Yi
      Nature Energy (2017), 2 (5), 17035CODEN: NEANFD; ISSN:2058-7546. (Nature Publishing Group)
      In contrast to conventional org. liq. electrolytes that have leakage, flammability and chem. stability issues, solid electrolytes are widely considered as a promising candidate for the development of next-generation safe lithium-ion batteries. In solid polymer electrolytes that contain polymers and lithium salts, inorg. nanoparticles are often used as fillers to improve electrochem. performance, structure stability, and mech. strength. However, such composite polymer electrolytes generally have low ionic cond. Here we report that a composite polymer electrolyte with well-aligned inorg. Li+-conductive nanowires exhibits an ionic cond. of 6.05 × 10-5 S cm-1 at 30 oC, which is one order of magnitude higher than previous polymer electrolytes with randomly aligned nanowires. The large cond. enhancement is ascribed to a fast ion-conducting pathway without crossing junctions on the surfaces of the aligned nanowires. Moreover, the long-term structural stability of the polymer electrolyte is also improved by the use of nanowires.
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  • Supporting Information

    Supporting Information

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmaterialslett.3c00538.

    • Experimental details, ionic conductivities of different filler materials, EIS, CV, SEM images, thermal stability of PP separator, cycle performance of NCM/Li half-cell, voltage profiles and cycle performance of LCO//Graphite pouch cell, and XPS spectra of BNNT before and after electrolyte exposure (PDF)


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