Journal of Energy Chemistry
·
2025
·
IF 14.9
Chenglong Yu,Shuyu Zhou,Pengpeng Dai,Tong Gao,Junhong Liao,Guozhong Cao,Shixi Zhao
The irreversible oxygen redox (OR) in Li-rich layered cathodes leads to severe structural degradation and voltage decay, particularly under harsh operating conditions. Although high-entropy oxides (HEOs) offer enhanced stability compared to conventional doping modifications, rational element selection for optimizing OR reversibility remains unexplored. Here, we propose an entropy engineering design paradigm for “oxygen-anchoring”, where optimal cation electronegativity (>Mn, 1.55) and d (3 d /4 d )- p orbital hybridization synergistically enhance transition metal–oxygen (TM–O) covalency and stabilize the O 2 p state. Two high-entropy Li-rich layered oxides: Li 1.2 Mn 0.47 Ni 0.115 Co 0.115 Mg 0.02 Ti 0.02 Al 0.02 Nb 0.02 Mo 0.02 O 2 (MTANM) and Li 1.2 Mn 0.47 Ni 0.115 Co 0.115 Mg 0.02 Ti 0.02 Cu 0.02 Nb 0.02 Mo 0.02 O 2 (MTCNM) were synthesized using partial nano-scale precursors and comparatively evaluated. MTCNM exhibits enhanced electrochemical performance and superior oxygen stability compared to MTANM by replacing Al with higher-electronegativity Cu, which possesses improved orbital overlap with oxygen. Both experiments and density functional theory (DFT) calculations demonstrate that element selection changes the covalency of TM–O through altered electronegativity and d orbitals- p orbitals ( d - p ) hybridization. Further stepwise screening selected the optimal elemental combination Li 1.2 Mn 0.47 Ni 0.115 Co 0.115 Cr 0.02 Cu 0.02 Nb 0.02 Mo 0.02 Ru 0.02 O 2 (CCNMR), which achieved near 100% capacity retention after 150 cycles at 1 C, 50 °C, with its voltage decay effectively suppressed. This work establishes a rational element-screening paradigm for entropy-stabilized OR chemistry in high-energy cathodes.
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DOI
高影响因子
ChemSusChem
·
2025
·
IF 6.6
Xinfeng Ma,Yiming Zhang,Wanlin Yang,Chengda Liu,Xin Wang,Yongzhu Fu
Organosulfur molecules are considered as highly promising cathode materials for lithium batteries due to their high theoretical specific capacities. However, their practical application is hindered due to the issues of the dissolution and shuttling of the discharge products as well as the electron/ion insulation. In this study, we synthesize abundant sulfur-vacancies niobium sulfide encapsulated by nitrogen-doped coral-shaped carbon (NbSx@N-CC) by an arc discharge method, and interweave it with carbon nanotubes (CNTs) to form an ideal host material for diphenyl tetrasulfide (PTS) as cathode in rechargeable lithium batteries. The NbSx@N-CC catalyst can accelerate the cathodic reaction kinetics, adsorb lithium polysulfides (LiPSs) to mitigate the shuttle effect, thus significantly improving the cycling performance. At the 0.5 C rate, the battery exhibits an initial discharge capacity of 520.7 mAh g−1, with a diminutive cycle capacity decay rate of 0.067% per cycle over 500 cycles. Even under the condition of high PTS loading (6.0 mg cm−2) and low electrolyte (5 μL mg−1), the Li-PTS battery can still maintain a capacity retention rate of 97% after stably cycling 150 times at 0.2 C rate. This work demonstrates that defect engineering is one of the effective approaches to address the challenges of lithium-organosulfur batteries.
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DOI
PubMed
高影响因子
DESALINATION
·
2025
·
IF 9.8
Ping Li,Yuan Zhou,Chunxi Hai,Ying Cheng,Yu Tang,Yanxia Sun,Shengde Dong,Luxiang Ma,Xin He,Qi Xu
Nanofiltration (NF) membranes prepared by traditional interface polymerization (IP) have garnered widespread attention for Mg 2+ /Li + separation. However, traditional NF membranes, like thin film composite polyamide (PA) membranes, show inadequate selectivity and permeance. The regulation of monomer diffusion plays a crucial role in adjusting the structure of nanofiltration membranes and improving their separation performance. In this study, we introduced the co-solvent N , N -dimethylformamide (DMF) into the aqueous phase to efficiently modulate the IP process of polyethyleneimine (PEI) and Trimesoyl chloride (TMC) without additional steps. The DMF-induced activation of the PA layer resulted in a more uniform pore structure across the layers, and the optimized membrane (CAIP (4)) had a pure water permeance of 13.10 ± 1.01 L/m 2 hbar, which was approximately three times that of conventional nanofiltration membranes. Molecular dynamics (MD) simulations indicated that the co-solvent DMF reduced the surface tension and accelerated the diffusion rate of PEI monomers, which diffused through the pores of the PA layer to leave more unreacted positively charged amine groups on the membrane surface. Consequently, the membrane achieved efficient separation of magnesium and lithium while maintaining good water permeance. The MgCl 2 removal was 95.09 % ± 1.65 %, and the Li + /Mg 2+ selectivity was 21.05. This study elucidates the mechanisms by which aqueous cosolvents influence IP reactions and offers novel strategies for modulating membrane structures and separation characteristics. These advancements are crucial for enhancing the efficiency of magnesium‑lithium separation processes.
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高影响因子
Joule
·
2017
·
IF 0
Fei Pei,Lele Lin,Ang Fu,Shiguang Mo,Daohui Ou,Xiaoliang Fang,Nanfeng Zheng
Summary Lithium-sulfur (Li-S) batteries are a promising next-generation energy-storage system due to their high theoretical energy density and low cost. However, the rapid capacity fading of high-sulfur-loading cathodes caused by the shuttle of soluble polysulfide intermediates between two electrodes heavily hinders the development of high-energy-density Li-S batteries. We develop in this work a powerful functional separator to suppress the polysulfide shuttle by coating two-dimensional nitrogen-doped porous carbon nanosheets on one surface of a commercial polypropylene separator. The high surface area, high content of nitrogen dopants, and close-packing laminar structure of the two-dimensional porous carbon nanosheets make them ideal to fabricate a lightweight and thin separator for high-energy-density Li-S batteries. The separator reported in this work endows the high-sulfur-loading cathodes made of commercial carbon materials with significantly enhanced performances that are comparable with or even superior to the state-of-the-art sulfur composite cathodes, opening up new opportunities for designing practical high-energy-density Li-S batteries.
研究领域:
材料科学
·
能源存储技术
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DOI
JOURNAL OF POWER SOURCES
·
2022
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IF 9.794
Zhidong Hou,Mingwei Jiang,Yunjing Cao,Huanyan Liu,Yu Zhang,Jian-Gan Wang
Developing high-capacity anode materials based on metal sulfides is of great importance for building advanced lithium-ion batteries (LIBs). Herein, we demonstrate rational encapsulation of cobalt sulfide (CoS x ) nanoparticles into multichannel carbon nanofibers (CoS x /MCF) with substantially improved Li + reactivity and durability. The unique multichannel and conductive carbon scaffold not only affords boosted electron/Li + transportation pathways for fast redox reaction with CoS x , but also stabilizes the electrode structure by buffering the volume change of CoS x . Impressively, the CoS x /MCF composite could serve as flexible anodes to deliver a high reversible capacity of 737 mAh g −1 at 0.2 A g −1 after 100 cycles, superior rate capacity of 374 mAh g −1 at 5 A g −1 , and excellent operating stability over 1000 cycles. Practical feasibility is also demonstrated by a full cell based on the high-capacity CoS x /MCF anode and Li[Ni 0.8 Co 0.1 Mn 0.1 ]O 2 cathode. The present study may provide insights for the facile synthesis of advanced anode materials for high-performance LIBs.
研究领域:
材料科学
·
能源存储
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DOI
高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Jiashi Liu,Jiacai Xiong,Yutao Xing,Chunhai Jiang,Zhimin Zou
Although silicon-based anode materials offer significantly higher specific capacity than graphite, their practical applications are limited by drawbacks such as large volume expansion, poor cycling stability and high production costs. Integrating transition metal oxides with silicon, coupled with a carbon coating layer, has been proven of effectiveness in enhancing the cycle stability of silicon-based anodes. Here we report the synthesis of a composite anode by combining tin(II) oxide (SnO) with waste silicon powder (wSi) of photovoltaic industry and introducing a carbon coating via in situ polymerization of resorcinol-formaldehyde followed by thermal pyrolysis. The resulting wSi/SnO@C composite anode exhibits improved rate and cycle performance, as characterized by a high reversible capacity of 1590 mAh g −1 at 3 A g −1 and a high retained capacity of 601 mAh g −1 after 500 cycles at 0.5 A g −1 . Mixing the wSi/SnO@C composite with graphite at an appropriate mass ratio yields a practical applicable anode with robust cycle stability. Ex situ X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses reveal that SnO is irreversibly reduced to metallic Sn during the first discharge, which is then partially converted to SnF 2 together with the formation of Li x Sn alloy. The formed SnF 2 is supposed to enhance the stability of the solid-electrolyte interphase (SEI) and reduce the attack of electrolyte to Si particles, both contributing to the improved cycle stability. This work demonstrates that SnO-decorated Si@C composites hold a high promise as anode materials of lithium-ion batteries towards enhanced cycle life and power density.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Peilin Ran,Xiaoqing Li,Kang Wu,Na Li,Kesheng Gao,Chenzhang Gu,Jinkui Zhao,Enyue Zhao,Zhimin Wu,Fangwei Wang
Cobalt-free Lithium-rich layered oxides (LRLOs) are promising cathodes for low-cost and high-energy-density Li-ion batteries. However, their remarkable capacity comes with challenges including structural degradation, irreversible oxygen release and sluggish kinetics. Herein, we conduct a one-step dual-modified strategy by yttrium doping and Li 3 PO 4 surface modification. Combining density-functional theory calculations with in-situ X-ray diffraction and in-situ differential electrochemical mass spectrometry, the Y 3+ doping and Li 3 PO 4 nano coating modified LRLOs is demonstrated has an excellent structural stability with enhanced Li⁺ diffusion kinetics and stabilized oxygen lattice. Excellent rate performance and thermal stability are achieved: high discharge specific capacity of 221 mAh·g −1 at room temperature (96.5 % at 1 C after 100 cycles) and incredible discharge specific capacity of 210 mAh·g −1 at 55 °C (91.8 % at 2 C after 100 cycles). This work resolves the safety and stability issues and provides a feasible strategy for Co-free LRLOs.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
Small
·
2023
·Vol. 19
·期 33
·2301275
·
IF 13.3
Huaxin Liu,Laiqiang Xu,Hanyu Tu,Zheng Luo,Fangjun Zhu,Wentao Deng,Guoqiang Zou,Hongshuai Hou,Xiaobo Ji
Solid-state polymer electrolytes are highly anticipated for next generation lithium ion batteries with enhanced safety and energy density. However, a major disadvantage of polymer electrolytes is their low ionic conductivity at room temperature. In order to enhance the ionic conductivity, here, graphene quantum dots (GQDs) are employed to improve the poly (ethylene oxide) (PEO) based electrolyte. Owing to the increased amorphous areas of PEO and mobility of Li + , GQDs modified composite polymer electrolytes achieved high ionic conductivity and favorable lithium ion transference numbers. Significantly, the abundant hydroxyl groups and amino groups originated from GQDs can serve as Lewis base sites and interact with lithium ions, thus promoting the dissociation of lithium salts and providing more ion pathways. Moreover, lithium dendrite is suppressed, associated with high transference number, enhanced mechanical properties and steady interface stability. It is further observed that all solid-state lithium batteries assembled with GQDs modified composite polymer electrolytes display excellent rate performance and cycling stability.
研究领域:
材料科学
·
电化学
·
能源存储
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Yixuan Guo,Jun Cheng,Zhen Zeng,Yuanyuan Li,Hongqiang Zhang,Deping Li,Lijie Ci
Garnet-type Li7La3Zr2O12 (LLZO) has been widely used as a filler in composite solid electrolytes (CSEs) to achieve high-performance solid-state batteries (SSBs). Unfortunately, moisture-sensitive LLZO suffers from surface Li2CO3 passivation when being exposed to an ambient atmosphere. The insulated Li2CO3 layer is thought to reduce the Li+ transportability of CSEs. However, further studies are still needed to find out the underlying mechanism, which helps to guide future filler modification and electrolyte design. Herein, the role of the Li2CO3 layer in CSEs is elucidated from different perspectives. The passivate Li2CO3 layer is verified to prohibit the formation of the high conductive interlayer, change the Li+ transport pathway, and decrease the carrier concentration in CSEs. Also, the Li2CO3 layer would reduce the electropositivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) particles, which therefore weakens the anchoring effect toward bis(trifluoromethanesulfonyl)imide (TFSI)−. Accordingly, without Li2CO3, the electrolyte of polyethylene oxide/LiTFSI/IL (ionic liquid) with LLZTO-AT (PLILA) displays 2 times higher ionic conductivity and an improved Li+ transference number of 0.49. Additionally, an excellent cycling performance is presented in Li symmetric cells and full cells with PLLA. This work provides a novel perspective for future research on lithium-ion transport mechanisms and inspires designing better-performance SSBs.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
Energy Sources Part A-Recovery Utilization and Environmental Effects
·
2022
·
IF 2.902
Bage Alhamdu Nuhu,Humphrey Adun,Olusola Bamisile,Mustapha Mukhtar
In this study, Ti-Fe-Si composites were prepared by one step ball-milling method as anode materials for Li-ion batteries. The effects of ball-milling speed and time were studied by X-ray diffraction, electron microscopy, and 57Fe Mössbauer spectroscopy. Changes in the composition and microstructure of the composites were observed and related to the electrochemical performance. Increasing ball-milling speed led to the formation of FeSix alloys that reduced the specific capacity while increasing the ball-milling time improved the particle size morphology and homogeneity. Discharge/charge profiles for the first two cycles were carried out at 0.05C current rate (1C = 1260 mAh.g−1for Li3.75Si). The first discharge for Ti-Fe-Si showed a LixSi reaction plateau of 1100 mAh.g−1, which were reversible and yielded columbic efficiency (CE) 77% and 90% in the first and second cycles, respectively. This capacity plateau indicated the insertion of about 3.25 Li into silicon. For the composite containing an additional 10% carbon SP, the theoretical capacity was about 1130 mAh.g−1, the discharge curve showed that the first discharge plateau reaches 1030 mAh.g−1 corresponding to 3.5 Li with the first CE was about 85%, and 98% for the second cycle. The addition of carbon to Ti-Fe-Si-C played a key role in capacity retention. The best results were obtained for the composite Fe/Ti/Si (1:1:2) with 10 wt% of carbon, ball-milled at 500 rpm for 48 hours. The specific capacities were about 900 mAh.g−1 at C/5 and 700 mAh.g−1 at 1C (C = 1200 mAg−1) with a capacity retention of about 90% for 100 cycles.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 9
Youran Xu,Rukang Tian,Hao Zhang,Xiaowen Wu,Yunkun Wang
The transition to renewable energy and the pursuit of carbon neutrality have heightened the demand for lithium extraction from salt lake brines to ensure a sufficient lithium supply. Nanofiltration (NF) membranes offer an efficient method for solute sieving; however, achieving highly selective Mg 2+ /Li + separation remains challenging due to their similar hydration radii. This study introduces a synergistic modification strategy to adjust the surface physicochemical properties of NF membranes through incorporation of a sodium alginate interlayer and post-treatment with piperazine. The resulting modifications improved Mg 2+ selectivity by optimizing steric and Donnan exclusion mechanisms, achieved through a refined pore size distribution and reduced surface negative potential. Consequently, the modified membrane exhibited an outstanding Mg/Li selectivity factor (>100), with Mg 2+ rejection efficiency exceeding 98%. The membrane also demonstrated stable performance under mixed feed conditions with high total dissolved solids (TDS, 2000 ppm) and low Li + concentration (100 MgCl 2 /LiCl mass ratio). This study provides a facile and effective approach to enhance multiple exclusion mechanisms for Mg 2+ separation, offering valuable insights into the design and fabrication of advanced NF membranes for efficient Mg/Li separation.
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高影响因子
SOLID STATE IONICS
·
2021
·
IF 3.785
Bo Fan,Zebo Guan,Hongjiao Wang,Lilin Wu,Wenzhi Li,Shibang Zhang,Bai Xue
Understanding the electrochemical processes in all-solid-state lithium‑sulfur batteries is essential for designing high-performance devices. Here, the evolution of the electrochemical impedance spectra of an all-solid-state lithium‑sulfur battery during one charge/discharge cycle was quantitatively investigated with a reasonably established equivalent circuit. The impedance spectra could be decomposed into several parts as follows: the bulk resistance of solid electrolyte and current collector at highest frequency, three semicircles from high to low frequency corresponding to the dynamic processes at different interfaces and a 45° straight line followed by an inclined small tail at low frequency. It is found that the middle frequency semicircle, corresponding to charge transfer at the cathode, varied obviously during the charge/discharge cycle. Moreover, the 45° straight line, which is attributed to the Li diffusion in the cathode material Li x S based on qualitative analysis, dominates the impedance spectra, revealing that the main kinetics-limiting factor is the Li diffusion in the active materials. Finally, an electrochemical model of the battery is proposed which provides insight for the designing of high-performance all-solid-state lithium‑sulfur batteries.
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高影响因子
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