Small
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2026
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IF 11.8
Gang Peng,Zhouyu Huang,Zhan Wu,Haiyuan Zhang,Dan Li,Wenlong Song,Yang Xia,Ruyi Fang,Wenkui Zhang,Xinyong Tao,Jun Zhang
Sulfide solid-state electrolytes (SEs) have emerged as promising electrolyte candidates for all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivity and excellent processability. However, the commercialization of sulfide SEs is hindered by the high cost of the essential Li 2 S raw material, making it difficult to strike a balance between high ionic conductivity and economic viability. In this study, we present a cost-effective synthetic approach based on anionic chemistry design to achieve both high ionic conductivity (2.53 mS cm −1 ) and low cost ($16.85/kg) for sulfide SSE. By replacing the conventional Li 2 S with low-cost precursors (LiH, S, and Li 2 O), the oxygen-substituted argyrodite SE is synthesized, while precisely engineering anionic lattice to effectively regulate lithium-ion transport dynamics. X-ray diffraction (XRD) Rietveld refinement and density functional theory (DFT) calculations reveal the crystal structure of the prepared Li 5.5 PS 3 O 1.5 Cl 1.5 and the origin of its high ionic conductivity. Moreover, LiNi 0.83 Co 0.12 Mn 0.05 O 2 (NCM 83 )/Li 5.5 PS 3 O 1.5 Cl 1.5 /Li ASSLB delivers more than 1000 cycles. Even under demanding conditions with a high active material loading of 10.7 mg cm −2 , the ASSLBs exhibit satisfactory electrochemical performance over 100 cycles. This strategy presents a novel and effective approach for preparing cost-effective and high-conductive sulfide SEs toward affordable ASSLBs.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xiaoxiao Liu,Qian Guo,Yu Li,Yue Ma,Xiaotao Ma,Panpan Liu,Donghong Duan,Zhonglin Zhang,Xianxian Zhou,Shibin Liu
The lithium-sulfur battery (Li-S) has been considered a promising energy storage system, however, in the practical application of Li-S batteries, considerable challenges remain. One challenge is the low kinetics involved in the conversion of Li 2 S 4 to Li 2 S. Here, we reveal that highly dispersed Ni nanoparticles play a unique role in the reduction of Li 2 S 4 . Ni-porous carbon (Ni-PC) decorated in situ on a free-standing carbon nanotube sponge (CNTS/Ni-PC) enriches the current response of liquid phase Li 2 S 4 and Li 2 S 2 around the cathode more than 8.1 and 5.7 times higher than that of the CNTS blank sample, respectively, greatly boosting the kinetics and decreasing the reaction overpotential of Li 2 S 4 reduction (lower Tafel slope and larger current response). Thus, with the same total overpotential, more space is provided for the concentration difference overpotential, allowing the more soluble polysulfide intermediates farther away from the surface of the conductive materials to be reduced based on the “wane and wax” strategy, and significantly improving the sulfur utilization. Consequently, S@CNTS/Ni-PC delivers excellent rate performance (812.4 mAh·g −1 at 2C) and a remarkable areal capacity of 10.1 mAh·cm −2 . This work provides a viable strategy for designing a target catalyst to enhance the conversion kinetics in the Li 2 S 4 reduction process.
研究领域:
材料科学
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电化学
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PubMed
高影响因子
Nature Catalysis
·
2023
·Vol. 6
·期 2
·174-184
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IF 37.8
Hua Wuxing,Shang Tongxin,Li Huan,Sun Yafei,Guo Yong,Xia Jingyi,Geng Chuannan,Hu Zhonghao,Peng Linkai,Han Zhiyuan,Zhang Chen,Lv Wei,Wan Ying
Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p -block metal sulfides and the apparent activation energies ( E a ) for the sulfur reduction reaction (SRR), in particular, Li 2 S n to Li 2 S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest E a and a high SRR rate in the cathode. Li–S batteries with the Bi 2 S 3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm −2 was obtained under a high sulfur loading of 17.6 mg cm −2 but a low electrolyte/sulfur ratio of 7.5 μl mg −1 .
研究领域:
材料科学
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电化学
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电池技术
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催化
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DOI
高影响因子
SOLID STATE IONICS
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2017
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IF 2.354
Qiang Zhang,Xiayin Yao,Jean Pierre Mwizerwa,Ning Huang,Hongli Wan,Zhen Huang,Xiaoxiong Xu
Transition metal sulfides have attracted particular interests owing to their extremely higher specific capacity and more compatible with sulfide electrolyte than lithium transition-metal oxide for all-solid-state lithium batteries. FeS nanosheets with thickness of 10 nm are synthesized by a poly (vinyl alcohol)-assisted precipitation method and further successfully employed in Li/70%Li 2 S-29%P 2 S 5 –1%P 2 O 5 /Li 10 GeP 2 S 12 /FeS all-solid-state lithium batteries. The obtained all-solid-state lithium batteries show reversible discharge capacity of 550 mAh g − 1 after 50 cycles at current density of 0.1 A g − 1 and exhibit superior rate performances.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Xiaotang Shi,Tianle Zheng,Jianwei Xiong,Bingying Zhu,Ya-Jun Cheng,Yonggao Xia
Increasing the working voltage of lithium-ion batteries (LIBs) is an efficient way to increase energy density. However, high voltage triggers excessive electrolyte decomposition at the electrode–electrolyte interfaces, where the electrochemical performance such as cyclic stability and rate capability is seriously deteriorated. A new synergistic positive and passive approach is proposed in this work to construct a stable electrode–electrolyte interface at high voltage. As a positive approach, inorganic lithium sulfide salt (Li2S) is used as an electrolyte additive to build a stable cathode electrolyte interface (CEI) at the LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode surface. In a passive way, acetonitrile (AN) is applied as a solvent additive to suppress oxidative decomposition of a carbonate electrolyte via preferential solvation with a lithium ion. Because of the synergistic interaction between the positive and passive approaches, the cyclic stabilities of NCM523/Li cells improved with a tiny amount of Li2S (0.01 mg mL–1) and AN (0.5 vol %). The capacity retention increased to 80.74% after 200 cycles compared to the cells with the blank electrolyte (67.98%) and AN-containing electrolyte (75.8%). What is more, the capacity retention of the NCM523/graphite full cell is increased from 65 to 81% with the addition of the same amount of Li2S and AN after 180 cycles. The mechanism is revealed on the basis of the theoretical calculations and various characterizations. The products derived from the preferential adsorption and oxidation of Li2S on the surface of NCM523 effectively increase the content of inorganic ingredients. However, the presence of AN prevents oxidation of the solvent. This study provides new principle guiding studies on a high-voltage lithium-ion battery with excellent electrochemical performance.
研究领域:
材料科学
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电化学
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能源存储
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PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Yeqiang Luo,Yepeng Fan,She Wang,Qiuyan Chen,Asad Ali,Jinliang Zhu,Pei Kang Shen
Lithium-sulfur (Li-S) batteries deliver a higher energy density than lithium ion batteries and are therefore regarded as next-generation batteries. However, the shuttle effect of soluble lithium polysulfides (LiPSs) and their slow redox kinetics are still the main setbacks for practical application. In this study, a porous three-dimensional carbon frame embedded with CoP nanoparticles (CoP@3DC) was synthesized by pyrolyzing and phosphating an acrylic cation exchange resin previously subjected to cobalt ion exchange. The abundant pores of CoP@3DC inhibit the diffusion of LiPSs, while its conductive three-dimensional carbon skeleton is conducive to the rapid transmission of electrons. In addition, CoP nanoparticles uniformly dispersed in the porous carbon network not only provide numerous chemical adsorption sites for LiPSs, but also accelerate their conversion to Li 2 S. Constant-current charging and discharging tests revealed that the CoP@3DC/S cathode achieves an initial discharge capacity of 1117.37 mAh∙g −1 at 0.5C and maintains a capacity of up to 740.56 mAh∙g −1 after 600 cycles, with a decay rate per cycle of only 0.056 %. Our work provides a facile supporting strategy for transition metal nanoparticles to significantly improve the performance of Li-S batteries.
研究领域:
材料科学
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能源存储
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电池技术
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DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2025
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IF 2.6
Cao Bo-Qun,Bao Hao-Tian,Zhang Ji-Wei,Shao Gang-Qin
The lithium-phosphorus-thiohalides (LPS X ) with superionic conduction are strong candidates for the new-generation solid electrolytes (SEs) in all-solid-state lithium-ion batteries (ASSLIBs). In this work, Li 6− x PS 5− x Cl 1+ x − y Br y (LPSCB; 0 ≤ x ≤ 0.7; 0 ≤ y ≤ 1.7) was synthesized by a solid-state method in which the key raw material of Li 2 S was prepared by an improved carbothermal reduction method without late decarbonization. The lattice flexibility and the degree of structural order are opposite effect and would lead to an optimum of the ionic conductivity at a composition of LPSCB. Li 6 PS 5 Br- and Li 5.5 PS 4.5 Br 1.5 -based ASSLIBs had the best rate capacity and cycle performance in Li 6 PS 5 Cl 1− y Br y - (0 ≤ y ≤ 1) and Li 5.5 PS 4.5 Cl 1.5− y Br y -based ones (0 ≤ y ≤ 1.5), respectively. To increase the ionic conductivity of LPSCB-type SEs and capacity/cycle performance of the related ASSLIBs, Br-introduction, mutual substitution and excess- X substitution were extremely effective strategies. Graphical
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高影响因子
JOURNAL OF POWER SOURCES
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2024
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IF 8.1
Zhanwei Xu,Jiaqi Zhao,Rongkun Lin,Jianfeng Huang,Xuetao Shen,Zhi Li
The shuttle and sluggish conversion kinetics of polysulfides (LiPS) significantly hinder the sulfur utilization and cycle performance of Li–S batteries. Herein, reduced Graphene Oxide supported Cobalt phthalocyanines(CoPc/rGO) and its skeleton Nitrogen substituent Cobalt Tetrapyridinoporphyrazine (CoTAP/rGO), are fabricated using a preform-solid synthesis process. When employed as separator modification, the CoTAP/rGO can capture and electrocatalyze LiPS by the active central Co–N 4 units. And the Co–N 4 sites are proved that can augment the LiPS redox kinetics especially the oxidation as well as the Li + diffusion rate. The introduced substituent N atoms in the skeleton match the LiPS redox ability and further enhance the Li + diffusion ability. Distribution of relaxation time (DRT) analysis shows that CoTAP nanoparticles can reduce the resistance of LiPS as well as Li + diffusion in Li 2 S precipitation procedure, accomplishing the loose three dimension deposition on cathode. As a result, the CoTAP/rGO separator exhibits a high initial capacity of 1132.7 mAh g −1 at 0.2C, excellent rate capacity of 672.5 mAh g −1 at 5C and superior long-term stability with a low capacity decay of 0.57 ‰ at 2C after 500 cycles.
研究领域:
材料科学
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电化学
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能源存储
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Zhongkai Wu,Ru Wang,Chuang Yu,Chaochao Wei,Shuai Chen,Cong Liao,Shijie Cheng,Jia Xie
Sulfide electrolytes show great potential as solid electrolytes for all-solid-state batteries due to their high ionic conductivity and low interfacial resistance toward electrode materials. The structure of the P–S framework in the composition of sulfides plays a crucial role in the conductivity. Introducing LiI in the Li3PS4 structure can tailor the P–S frameworks and thus achieve high ionic conductivities. Herein, the dopant of LiI is optimized by high-rotation milling, followed by a sintering route to achieve the highest Li-ion conductivity of 2.3 mS cm–1 for the Li3PS4-50% LiI electrolyte (also denoted as Li7P2S8I) among different compositions. The phase variations and structure evolution of the P–S frameworks in the LiI-doped Li3PS4 electrolytes are carefully investigated in a combination of X-ray diffraction and Raman spectra. All-solid-state Li–S batteries using the prepared Li7P2S8I electrolyte combined with a nano Li2S cathode and a Li–In anode deliver a high initial discharge capacity of 739.7 mA h g–1 and sustain a discharge capacity of 517.7 mA h g–1 after 60 cycles with a capacity retention of 70.0% at 0.13 mA cm–2 at room temperature. When the operating temperature rises to 60 °C, it shows a higher discharge capacity of 862.8 mA h g–1 with fast capacity decay. However, it exhibits stable capacities and superior cycling performance under 0 °C over 70 cycles. Electrochemical impedance spectroscopy and in situ stack-pressure results find that the electrochemical performance differences of the assembled battery at different operating temperatures are associated with the interfacial resistance caused by volume changes. This work provides the strategy to obtain highly conductive sulfide electrolytes for SSBs and unravels the temperature effects on the electrochemical performance of all-solid-state Li–S batteries.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
NEW CARBON MATERIALS
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2023
·
IF 5.7
Xian-lan Ke,Yu-heng Lu,Jin-lun Wu,Ding-cai Wu
We report the fabrication of vulcanized cross-linked polystyrene grafted on carbon nanotubes (CNTs) for use as an advanced three-dimensional Li host. First, polystyrene was grafted from Br-modified CNTs to form brush-like structure by surface-initiated atom-transfer radical polymerization. Polystyrene grafted on carbon nanotubes was then cross-linked using a Friedel-Crafts reaction and finally vulcanized with sulfur. Vulcanized cross-linked polystyrene grafted on carbon nanotubes was used as a support for the Li metal, and its macro-, meso- and microporous structure increased Li ion transport, buffered the volume changes of the Li anode, and provided a high specific surface area to reduce local current density, which assisted rapid and uniform Li plating/stripping. At the same time, the homogenously distributed sulfur in the support reacted with Li to produce a Li 2 S-containing SEI layer, while the CNTs provided conductive pathways for the rapid transmission of electrons. As a result, a Li|Li symmetric cell using this anode material and a Cu current collector had a stable cycling performance of more than 500 h at a current density of 1 mA cm −2 . When LiFePO 4 was used as the cathode, a full cell had a high discharge capacity of 101 mAh g −1 with a capacity retention of 77% after 600 cycles at 1 C.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）