Separations
·
2026
·Vol. 13
·期 6
·163
·
IF 3.5
Jingyi Wang,Yu Zhang,Lingen Zhang
Spent lithium-ion battery electrolytes contain fluorine-, sulfur-, and phosphorus-bearing toxins, necessitating deep detoxification and directional conversion into C1–C6light hydrocarbons. To elucidate the specific catalytic roles and sequential activation of cathode metals (Li, Ni, Co, Mn), this work systematically deconvolutes their mono- and multi-metallic migration mechanisms over a CaO-ZSM-5* catalyst during vacuum catalytic pyrolysis (530 °C, 100 Pa). Results reveal that Li+and Ni2+dominate C–O bond cleavage in carbonates and CaO-ZSM-5*-assisted decarboxylation and oxygen fixation, significantly increasing the relative hydrocarbon content. Conversely, Co2/3+and Mn4+release reactive oxygen species, causing deep oxidation of hydrocarbons into CO2and antagonizing the targeted conversion. In multi-metallic systems, forming composite metal oxides (MxNyOz) increases the energy barrier for releasing active catalytic ions, hindering carbonate cleavage and leaving unreacted carbonate feedstocks. For detoxification, F and P are effectively immobilized as CaF2and Ca2P2O7. The relative content of detected gas-phase nitriles is minimized to <2% due to the strong antagonistic effect of Ni2+on Li+-promoted hexanedinitrile cleavage, while sulfur species derived from 1,3-propane sultone are converted to SO2and ultimately mineralized as calcium and metal-sulfur salts. Mechanistically, product distributions and crystallographic properties suggest a hypothesized sequential activation model—Li+→ Ni2+→ Mn4+—governing reactivity, whereas Co2/3+does not participate in the synergistic detoxification and selective upgrading process. This migration–reaction coupling framework provides critical insights for cathode-assisted in situ catalytic pyrolysis and closed-loop electrolyte recycling.
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Chao Yue Zhang,Guo Wen Sun,Zu De Shi,Qian Yu Liu,Jiang Long Pan,Yan Chun Wang,Hao Zhao,Geng Zhi Sun,Xiu Ping Gao,Xiao Jun Pan,Jin Yuan Zhou
Atom-intercalated transition metal disulfides (TMDs) have attached much attention mainly due to their highly improved conductivity. But it is few reported that the atom intercalation can enable the TMDs have unexpected catalytic properties, caused by the unit-cell deformation in them. In this work, a type of V 0.25 -intercalated VS 2 (V 5 S 8 ) nanoflakes was designed via a direct vulcanization method combining Kirkendall heat diffusion effect, and used as the promotor for lithium-sulfur batteries (LSBs). The V 5 S 8 possesses a NiAs crystal structure, in which V atoms occupy the interlayer spacing between VS 2 monolayers, which will unavoidably cause the unit-cell deformation. As expected, the CNF@V 5 S 8 /S cathodes show a specific capacity of 1260 mAh g −1 at 0.2 C, and can keep 73.65% of the capacity with charge/discharge rate increasing 10 times; while the CNF@VS 2 /S ones can only retain 54.0% of the initial capacity. Moreover, the CNF@V 5 S 8 /S cathodes show an ultralow decay rate of only 0.0312% per cycle for 1500 cycles at 5 C. Furthermore, the catalysis effect of V 5 S 8 on the conversion of lithium polysulfide (Li 2 S n , n = 1, 2, 4, 6 and 8) and S 8 clusters were systematically discusses. Besides, the V 5 S 8 can further enable LSBs achieve a high areal capacity (8.2 mAh cm −2 with sulfur loading of 7.8 mg cm −2 ) and a high dynamic flexible stability at bending angle between 0 and 180 °.
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高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 42
·22065-22074
·
IF 11.301
Hongling Guo,Gang Wang,Rutao Meng,Yali Sun,Siyu Wang,Shengli Zhang,Jianyu Wu,Li Wu,Guangxing Liang,Hui Li,Yi Zhang
A Li+-doping strategy is a promising route for achieving highly efficient Cu2ZnSn(S,Se)4 (CZTSSe) photovoltaic devices with a large grain absorber layer, high p-type carrier concentration and good band alignment at the Cu2ZnSn(S,Se)4/CdS interface. However, Li+-doped CZTSSe solar cells based on in situ and pre-deposition doping strategies reported thus far generally suffer from massive lithium losses and sodium rejection due to the soda-lime glass substrate. Therefore, simultaneously fulfilling the goals of simple and efficient Li+-doping remains a major technical challenge, which may be addressed, as we demonstrate here, with the development of a Se&LiF co-selenization process. By engineering the band alignment of the Cu2ZnSn(S,Se)4/CdS interface through the Se&LiF co-selenization process, an encouraging efficiency of 11.63% with an open-circuit voltage deficit of 0.583 V has been reached. Furthermore, the crystallinity of the absorber layer and the distribution of copper are improved, and a more copper-poor CZTSSe surface is formed. This novel Li+-doping strategy introduces a new approach towards the goal of high-performance CZTSSe solar cells compatible with a simple manufacturing process and excellent performance.
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高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Jinlong Cui,Haibang Zhang,Yunying Liu,Shaohui Li,Wenxiu He,Jiangliang Hu,Juncai Sun
To enhance electrochemical properties of C/SiO x composite for business application, N-doped carbon/SiO x composite has been successfully fabricated using rice husks as the raw material of both C and Si sources and urea as N source via an environmentally friendly and economically viable strategy. The obtained N@C/SiO x composite exhibits a porous irregular particle morphology with a high specific surface area. SiO x particles are uniformly dispersed in N-doped C skeleton. As an anode material for Li-ion batteries, the porous structure, N doping and high reduction degree of SiO 2 endow N@C/SiO x electrodes with an outstanding reversible capacity up to 1018.5 mAh/g at 0.1 A/g and a remarkable initial coulombic efficiency of 72.2%, which is larger than that of carbonized rice husks (45.7%). Even if the current density rises to 1.0 A/g, the reversible specific capacity can maintain at 623.3 mAh/g with a capacity degradation of merely 4.0% after 1000 cycles.
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高影响因子
JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 24
·3276-3287
·
IF 3.4
Jinglei Xing,Ge Zhu,Xingzhong Fang,Guofei Chen
To meet the needs of high heat-resistant and colorless polyimide (CPI) films, a series of poly(amide-imide) (PAI) films were synthesized by copolymerization of 1,2,3,4-cyclobutanetetracarboxylic dianhydride (CBDA), terephthaloyl chloride (TPC), 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) and 2,2′-bis(trifluoromethyl)benzidine (TFDB) with the addition of lithium chloride (LiCl) for ionic coordination. The coordination of Li cations with carbonyl groups significantly reduced the coefficient of thermal expansion (CTE) and improved the mechanical properties. Moreover, by adjusting the ratio of CBDA and TPC, all PAI films exhibited high glass transition temperature ( T g ), low CTE and high transparency. Among these PAI films, PAI-6-2Li exhibited excellent comprehensive performance with a high T g of 363 °C, low CTE of 6.4 ppm/K, high transmittance of 84% at 400 nm and tensile modulus of 7.2 GPa, which was expected to be used in the field of flexible displays. Graphical
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高影响因子
POLYMER
·
2023
·
IF 4.6
Jingjing Hou,Lu Han,Shuzheng Sun,Mingkai Li,Junbo Yue,Yanqin Yang,Jingde Li
The commercialization of lithium-sulfur (Li-S) batteries has been restrained mainly by lithium polysulfides (LiPSs) shuttling and sluggish electrochemical reactions . Herein, a functional separator with synergy effect between adsorption and catalysis is proposed to solve the above problems. Specifically, an ultrathin barrier layer of a functionalized intrinsic microporous polymer (Li-AOPIM-1) is coated on SWCNT gutter layer through spin coating and applied to modify the cathode side of commercial polypropylene (PP) separator. In this configuration, the robust SWCNT gutter layer with high conductivity can not only work as a physical barrier to block the macropores of PP separator, but also improve the integral conductivity, resulting in a rapid charge migration and reaction kinetics. The electronegative heteroatoms N and O in Li-AOPIM-1 top layer have strong adsorption capability to LiPSs so that modified separator can restrain the shuttle effect admirably. Moreover, the introduction of lithiated sites further enhance the lithium-ion conductivity. Accordingly, the Li-S batteries implementing this modified separator deliver stable lifespan with only 0.062% capacity fading rate per cycle after 500 cycles at 1 C and superior rate performance of 700.6 mAh g −1 at 3 C. This work will provide a feasible strategy for the practical applications of high-performance Li-S batteries.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Xiaolan Chen,Tian Wang,Wanzheng Lu,Tianxiang Cao,Mingzhe Xue,Bing Li,Cunman Zhang
A modified solution method was applied to synthesize cubic garnet solid-state electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) and Li 6.45 Ca 0.05 La 2.95 Ta 0.6 Zr 1.4 O 12 (LCLTZO). The synergetic doping of Ca and Ta is found to induce the formation of cubic LCLZTO with high ionic conductivity of 4.03 × 10 −4 S cm −1 while LLZO without substitution exhibits tetragonal phase with low conductivity. A Li-S cell with sulfur cathode and as-prepared LCLTZO solid electrolyte “separator” was conducted to deliver large initial discharge capacity of 1090 mAh g −1 with high initial Coulombic efficiency up to 92%. Cell with LCLTZO also exhibited better cycling performance at 0.2 C and extremely high Coulombic efficiency (close to 100%) than the cell without solid electrolyte. Better rate performance was also achieved at lower rate (0.2 C, 0.5 C and 1 C) by cell with LCLTZO although it lost advantages at higher rate of 2 C and 5 C due to the limitation of ionic conductivity of LCLTZO. Energy dispersive X-ray spectroscopy (EDS) provided direct evidence that LCLTZO solid electrolyte greatly suppressed the shuttle effect generated by polysulfides . The electrochemical impedance spectroscopy was applied to discuss the difference between cells with and without LCLTZO during the discharge process. Charge transfer reaction referred to soluble polysulfides was found to be slower in cell with LCLTZO than that in cell without solid electrolyte.
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高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Guiru Sun,Qin Zhao,Tong Wu,Wei Lu,Mei Bao,Liqun Sun,Haiming Xie,Jia Liu
The development of self-standing and binder-free O2 electrodes is significant for enhancing the total specific energy density and suppressing parasitic reactions for Li–O2 batteries, which is still a formidable challenge thus far. Here, a three-dimensional foam-like composite composed of Mo2C nanorods decorated by different amounts of N-doped carbon (Mo2C-NR@xNC (x = 5, 11, and 16 wt %)) was directly employed as the O2 electrode without applications of any binders and current collectors. Mo2C-NR@xNC presents a network microstructure with interconnected macropore and mesoporous channels, which is beneficial to achieving fast Li+ migration and O2 diffusion, facilitating the electrolyte impregnation, and providing enough space for Li2O2 storage. Additionally, the coated N-doped carbon layer can largely improve the electrochemical stability and conductivity of Mo2C. The cell with Mo2C-NR@11NC shows a considerable cyclability of 200 cycles with an overpotential of 0.28 V in the first cycle at a constant current density of 100 mA g–1, a superior reversibility associated with the formation and decomposition of Li2O2 as desired, and a high electrochemical stability. On the basis of the experimental results, the electrochemical mechanism for the cell using Mo2C-NR@11NC is proposed. These results represent a promising process in the development of a self-standing and binder-free foam-based electrode for Li–O2 batteries.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 23
·10856-10867
·
IF 9.931
Xiangzhong Ren,Moujie Huang,Shan Luo,Yongliang Li,Libo Deng,Hongwei Mi,Lingna Sun,Peixin Zhang
A novel free-standing and binder-free air electrode with excellent electrochemical performance was designed for highly reversible Li–O2 batteries. The 3D hierarchically N, S co-doped macro–mesoporous carbon (NSMmC) was deposited on carbon paper (CP) via a template method, and then uniformly decorated with PdNi nanoparticles. The macropores of the porous carbon can provide enough space to accommodate discharge products, while the interconnected pores and channels efficiently facilitate oxygen and electrolyte diffusion. The introduction of PdNi nanoparticles greatly reduce the charge transfer resistance, resulting in the improvement of electron mobility of the whole cathode. Compared with Pd–NSMmC/CP and NSMmC/CP cathodes, the PdNi–NSMmC/CP cathode shows considerable enhancement of Li–O2 battery performance. The ultrafine and evenly distributed PdNi nanoparticles can not only provide enough catalytic sites, but can also tailor the discharge products into a cage-like morphology, which provides enough channels for electron and lithium ion transport. Moreover, the smaller size of the cage-like Li2O2 makes it decompose more easily, resulting in lower charge overpotential. This study provides a promising strategy to design 3D structured air cathodes for Li–O2 batteries with high electrocatalytic performance.
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高影响因子
RSC Advances
·
2016
·Vol. 6
·期 13
·10824-10830
·
IF 3.289
Zerui Chen,Jianfei Zhou,Xiaoling Wang,Xuepin Liao,Xin Huang,Bi Shi
A C@Fe3O4 core–shell nanofiber bundle (C@Fe3O4NFB) was easily prepared using a natural collagen fiber (CF) as the biotemplate and carbon source. The as-prepared C@Fe3O4NFB features a continuous conductive pathway with dramatically accelerated electron and Li+ transport kinetics, thus exhibiting an ultrahigh-rate capability. Furthermore, the C@Fe3O4 core–shell structure is able to suppress the electrode pulverization due to the existence of the carbon nanofiber as an elastic buffering matrix, thus delivering long-term cycling stability. Based on electrochemical experiments, C@Fe3O4NFB delivered capacities of 839, 668, 422 and 301 mA h g−1 at current densities of 0.2, 1.0, 5.0 and 10.0 A g−1, respectively. At the current density of 1.0 A g−1, the reversible capacity of C@Fe3O4NFB is as high as 632 mA h g−1 in the 500th cycle, which accounts for 84.38% capacity of the 2nd cycle, suggesting a low capacity loss of 0.23 mA h g−1 per cycle. Even after 2000 cycles at 5.0 A g−1, the discharge capacity still reaches 354 mA h g−1. This biotemplated synthesis approach provides a novel and interesting route for fabricating ultrahigh-rate anode materials of LIBs.
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高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Y. Zhang,X. Lou,J. Dan,C. Franke,L. Tang,J. Li,Z. Gao,L. Zhou,B. Chen,T. Li,T. Liu
All-solid-state lithium batteries with lean (ultrathin) lithium anodes and polymer-based electrolytes e.g., polyethylene oxide (PEO), can potentially offer high energy density , reduced processing cost and improved mechanical contact at electrolyte-electrode interfaces. The non-uniform lithium deposition and inadequate mechanical strength of PEO, however, tend to cause deactivated lithium and short-circuiting by Li dendrites over lithium deposition/stripping cycles; these issues become more aggravated with lean Li anodes due to the more severe volume changes. Herein, we construct a more mechanically and chemically stable lithium-electrolyte interface by coupling alloyed lean Li anodes (<50 μm) with PEO electrolytes blended with polymers of intrinsic porosity (PIMs). The lean Li anode is fabricated by a facile and scalable cold-rolling method, which leads to a uniformly alloyed lithium anode permitting epitaxial Li deposition. Meanwhile, PIM reinforces the mechanical strength of the PEO composite electrolyte, reducing the likelihood of dendrite formation/penetration. Importantly, the introduction of both GaInSnZn and the first-generation PIM has been found to reduce the interfacial charge transfer resistance via modifying the composition of solid-electrolyte interphase. The resulting full cells with lithium iron phosphate cathodes exhibit a high specific capacity of ∼160 mAh/g, i.e., ∼0.6 mAh/cm 2 with excellent retention of 93.1 % at 120 cycles.
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高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Zhao-Lei Huo,Jia-Yu Qiao,Le-Xi Zhang,Yao-Wen Yue,Qi-Da Qiu,Zhi-Jiang Hou,Jing Yin,Li-Jian Bie
Nowadays, attractive progress has been made on flexible humidity sensors for multifunctional applications, yet most of them still suffer from intrinsic instability due to the device structure based on flexible substrates. Herein, high-performance flexible humidity sensors were constructed using alkali metal halide doped polyvinylpyrrolidone (PVP)/polyvinylidene fluoride (PVDF) freestanding films. These films are prepared via a versatile thermally induced phase separation procedure with a network-like porous structure. After doping with metal salts of MCl (M = Li, Na, K), the humidity sensing performance is highly improved, among which the LiCl@PVP/PVDF film is the optimized one. In the relative humidity range of 11–97% at room temperature, the LiCl@PVP/PVDF sensor exhibits high response (2.3 × 103), fast response (10 s), small hysteresis (0.41%), and excellent repeatability. Notably, the LiCl@PVP/PVDF film is featured as fully self-supporting without the assistance of any substrate, readily tailorable that can be cut into different shapes, as well as highly flexible that can be bent to certain angles, and meanwhile almost maintains its response without significant decrease. Furthermore, the excellent performance enables the LiCl@PVP/PVDF sensor to demonstrate great potential in real-time noncontact diaper and finger detection. This contribution provides a practical humidity sensing candidate for moisture monitoring and gives insights into the fields of humidity sensors and flexible electronics.
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高影响因子
危险品化学品经营许可证（带存储）