ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Shuo Wang,Yibo Zhang,Xue Zhang,Ting Liu,Yuan-Hua Lin,Yang Shen,Liangliang Li,Ce-Wen Nan
Highly Li-ion conductive Li6PS5Cl solid-state electrolytes (SSEs) were prepared by solid-state sintering method. The influence of sintering temperature and duration on the phase, ionic conductivity, and activation energy of Li6PS5Cl was systematically investigated. The Li6PS5Cl electrolyte with a high ionic conductivity of 3.15 × 10–3 S cm–1 at room temperature (RT) was obtained by sintering at 550 °C for just 10 min, which was more efficient taking into account such a short preparation time in comparison with other reported methods to synthesize Li6PS5Cl SSEs. All-solid-state lithium sulfur batteries (ASSLSBs) based on the Li6PS5Cl SSE were assembled by using the nano-sulfur/multiwall carbon nanotube composite combined with Li6PS5Cl as the cathode and Li–In alloy as the anode. The cell delivered a high discharge capacity of 1850 mAh g–1 at RT for the first full cycle at 0.176 mA cm–2 (∼0.1C). The discharge capacity was 1393 mAh g–1 after 50 cycles. In addition, the Coulombic efficiency remained nearly 100% during galvanostatic cycling. The experimental data showed that Li6PS5Cl was a good candidate for the SSE used in ASSLSBs.
研究领域:
材料科学
·
电化学
·
储能
·
固态电池
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Junmin Ke,Mengru Wu,Han Bao,Jianghao Zhao,Furong Liu,Guofeng Xu
All-solid-state batteries (ASSBs) with lithium metal anodes are expected to be one of the most promising energy storage systems to achieve high energy density. However, the interfacial side reactions between lithium anodes and argyrodite electrolytes significantly limit the cycling stability. Herein, a self-adaptive Li–Mg–Cl interphase is constructed in situ through driving the MgCl2 incorporated Li6PS5Cl with an electric field. Ab initio molecular dynamics (AIMD) analysis reveals that the Li–Mg–Cl network undergoes dynamic covalent-ionic bond reorganization, enabling self-anchored interfacial coordination of Li–Mg, Li–Cl, and Mg–Cl. The dynamic bonding of Li–Mg–Cl further exhibits self-healing behavior due to lithophile site, which autonomously repairs structural defects during the (de)lithiation process. Moreover, the interphase regulation inhibits dendrite formation through improving the mobility of Li+ ions. Consequently, the assembled cell operates stably for 1300 h under a current density of 0.1 mA cm–2 at 25 °C. The all-solid-state batteries with LiNi0.8Co0.1Mn0.1O2 as cathode demonstrate outstanding performance, with an initial capacity of 169 mAh g–1 at 0.2 C and a capacity retention of 80% after 100 cycles. The electrolyte modified with an electric field, based on its low-cost and highly energy-efficient features, further promotes the development of sustainable production processes.
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2026
·
IF 20.2
Xin Gao,Ya Chen,Bin Fang,Xiaodong Chen,Runjing Xu,Tao Meng,Ling Huang,Peiyi Ji,Long Bao,Hongchao Sun,Lifeng Cui,Gang Tan,Guoxiu Wang
The electrochemical performance of all-solid-state lithium batteries (ASSLBs) can be markedly enhanced by resolving issues arising from cathode conductive additives (CCAs), including excessively high interfacial impedance, inadequate compatibility with solid electrolytes, and insufficient adaptability to the composite cathode. Here, the embedding of ultra-thin and ultra-stable MoS 0.25 Se 1.75 nanosheets onto a vapor-grown carbon fibers (VGCF) substrate are successfully fabricated (MoS 0.25 Se 1.75 @VGCF) as CCAs within a LiCoO 2 -based composite cathode for Li 6 PS 5 Cl (LPSC)-based ASSLBs. This advanced nanostructure design not only effectively suppresses the presence of hydroxyl groups (-OH) on the surface but also induces a synergistic effect that builds up a strong internal electric field and simultaneously lowers the Li + ions migration energy barrier, which can mitigate the occurrence of LPSC degradation at the CCAs|LPSC interface while establishing dual electron/Li + ion transport pathway, thus strengthening the compatibility of composites cathode interfaces for the improvement of electrochemical performance. Consequently, the assembled LCO|MoS 0.25 Se 1.75 @VGCF|LPSC-based ASSLBs exhibit exceptional performance, demonstrating a high discharge capacity of 131.24 mAh·g -1 at 0.1C, a high coulombic efficiency of 92.34%, and an excellent capacity retention of 90.41% after 1000 cycles at 0.5C. This finding introduces a novel synergistic strategy, which offers a fresh approach to mitigate interfacial instability in composite cathodes, thereby further facilitating the commercialization of ASSLBs.
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产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2021
·Vol. 8
·期 15
·2100624
·
IF 6.147
Zhen Sun,Yanqing Lai,Na lv,Yaqi Hu,Bingqin Li,Shenghao Jing,Liangxing Jiang,Ming Jia,Jie Li,Shiyou Chen,Fangyang Liu
Solid-state batteries exhibit promising prospects due to their potential in terms of safety and energy density. Sulfide solid electrolytes have received much attention due to their high ionic conductivity (about 10 −2 S cm −1 ). However, high side reactions between solid sulfide electrolytes and oxide cathodes, such as LiCoO 2 , have hampered the development of all-solid-state sulfide batteries. Here, first-principles calculations and experiments are combined to demonstrate a novel protective layer to cope with the Li 6 PS 5 Cl electrolyte and LiCoO 2 cathode interface problem. By uniformly coating LiCoO 2 with a layer of Li 2 WO 4 , the interfacial resistance (the 100th cycle) between the sulfide electrolyte and LiCoO 2 is reduced to about 68 Ω cm 2 , which is nearly 15 times lower than the premodified 1061 Ω cm 2 . The 2 wt% Li 2 WO 4 -coated LiCoO 2 (2%LWO-LCO)/Li 6 PS 5 Cl/Li-In all-solid-state battery exhibits satisfactory capacity and excellent cycling stability at room temperature (93% capacity retention after 100 cycles). Furthermore, the ab initio molecular dynamics based on the Perdew, Burke, and Ernzerhof density functional theory calculations show that Li 2 WO 4 can effectively prevent the diffusion of Co and O from LiCoO 2 into the Li 6 PS 5 Cl solid electrolyte. It is shown that molecular dynamics help predict the interfacial reactions in all-solid-state sulfide batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Zhigao Luo,Xianyou Wang
All-solid-state lithium metal batteries (ASSLMBs) with argyrodite-type Li6PS5Cl solid electrolyte (SE) show potential to replace current commercially available lithium-ion batteries by virtue of their potentially high energy density and safety. However, the interface incompatibility between sulfide solid electrolyte and lithium metal leads to an increase in interfacial resistance and the rapid growth of lithium dendrites, which greatly impede its commercial application. To alleviate the above problems, here a cell construction model has been put forward, in which composite polymer electrolytes (CPEs) with high ionic conductivity and good interface compatibility against lithium metal are employed as the interphase between Li6PS5Cl solid electrolyte and lithium metal. CPEs can prevent direct contact between lithium anode and Li6PS5Cl, and a soft CPE layer can solve the problem of high interfacial resistance caused by bad contact between the Li6PS5Cl solid electrolyte and the lithium metal anode. As a result, the symmetric cells Li/CPEs/Li6PS5Cl/CPEs/Li show stable polarization voltage over 140 h at a current density of 0.2 mA at 60 °C. Compared with the rapidly decaying capacity of the LiFePO4/Li6PS5Cl/Li cell, the initial discharge capacity of LiFePO4/Li6PS5Cl/CPEs/Li is 93.74 mAh/g, and after 15 cycles at 0.5 C, the capacity retention rate is still 75.1%. Therefore, the successful design of this cell structure based on the interface modification of Li6PS5Cl solid electrolyte provides good prospects for the commercial application of ASSLMBs.
研究领域:
材料科学
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电化学
·
能源存储
·
固体离子学
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电池技术
·
界面工程
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 24
·2214274
·
IF 19
Shenghao Jing,Huaqing Shen,Yuting Huang,Wuqi Kuang,Zongliang Zhang,Siliang Liu,Shuo Yin,Yanqing Lai,Fangyang Liu
Sulfide-based all-solid-state batteries (ASSBs) have a wide application prospect because of the advantages of higher energy density and better intrinsic safety over conventional lithium-ion batteries (LIBs). The compatibility of sulfide-based electrolytes with various organic solvents and the possibilities of the slurry coating process with these systems remain veiled that limits the large-scale fabrication of sulfide-based ASSBs. In this study, polyvinylidene fluoride (PVDF) binder and isobutyl isobutyrate (IBB) are selected as the combination of binder and solvent to achieve scalable slurry process after examining the chemical and electrochemical compatibility of Li 6 PS 5 Cl (LPSC) solid electrolyte, PVDF, and IBB. A comparative investigation of sheet-type LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) electrodes and pellet-type NCM811 electrodes shows that PVDF hinders the transport of Li + and electron, but it benignantly works as a buffer layer, which alleviates the side reaction in the composite cathode electrode. Further, PVDF is modified by LiClO 4 to facilitate interfacial Li + transport, which improves the capacity retention of the cell at 0.5 C to 97.05% after 100 cycles. Finally, NCM811/graphite full-cell is successfully fabricated by the slurry coating process, which demonstrates the feasibility of practical and scalable fabrication of sulfide-based ASSBs with slurry process and its performance enhancement effect via LiClO 4 modification.
研究领域:
材料科学
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电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Bingqin Li,Zhen Sun,Na Lv,Yaqi Hu,Liangxing Jiang,Zongliang Zhang,Fangyang Liu
All-solid-state lithium metal batteries (ASSLMBs) are considered promising candidates for next-generation energy storage systems. However, the growth of Li dendrites and interface side reactions hinder the practical application of ASSLMBs. To address these issues, a preformed Li–Ag alloy anode for an ASSLMB with the Li6PS5Cl electrolyte was constructed. The preformed Li–Ag alloy anode contains two distinct alloy layers, i.e., Li3Ag and Li0.98Ag0.02, with the former as a protection layer and the latter as a Li deposition site. Besides, a beneficial stable interlayer (Ag–P–S–Cl compound) produced by the reaction between Ag and Li6PS5Cl could work as a secondary protection layer between the anode and electrolyte. The dual protection (Li3Ag and Ag–P–S–Cl compound) suppresses dendritic growth and other interfacial issues effectively and simultaneously. Consequently, a LiCoO2/Li6PS5Cl/Li–Ag all-solid-state battery exhibits a remarkable specific capacity and excellent cycle stability. The dual-protection effect from the preformed Li–Ag alloy anode and the investigation of its working mechanism may enlighten a simple strategy for promoting the development of ASSLMBs.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Minghao Zhang,Shaojian Zhang,Chenyu Liu,Zengqing Zhuo,Yuan Lei,Denghai Xiao,Chenghao Yao,Wei Fu,Chunni Jiang,Yiting Miao,Li Feng,Zhan Lin
All-solid-state lithium-ion batteries (ASSLIBs) with many advantages are excellent candidates for eVTOL batteries. However, a significant challenge arises from the incompatibility between cathode materials and sulfide solid-state electrolytes (S-SSEs). To overcome this, a sulphuration reduction interphase consisting of CoO/Li 2 SO 4 /Li 2 CO 3 is formed on the surface of the cathode through a simplified sulfur-induced thermal reduction process applied to lithium cobalt oxide (LCO) in this work. The introduction of sulfur transforms the LCO surface, enhancing compatibility with S-SSEs. Consequently, ASSLIBs exhibit a notable initial capacity of 143.3 mAh g −1 at 0.2 C, with 86.19 % capacity retention after 200 cycles. Furthermore, the batteries in this study demonstrate an outstanding rate capacity of 77 mAh g −1 at 2 C (pristine sample with 0 mAh g −1 at 2 C). This evidence strongly substantiates the remarkable efficacy of the sulphuration reduction interphase in effectively mitigating interfacial reactions and ensuring rate ability. Essentially, this study opens new avenues for fostering a stable cathode/SSEs interface, providing a novel framework for designing high-performance and safe eVTOL batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Liu Chong,Wang Ruoyu,Wang Dewen,Zhao Liyun,Li Taiguang,Wang Tenghui,Chen Butian,Zhang Tianran,Liu Xiangfeng
Sulfides-based all-solid-state lithium batteries show great potential due to their high safety and high energy density, yet severely suffer from sulfide electrolytes/Li interfacial instability and short cycle life. Here we propose a Li-In-S composite foil comprising Li 2 S, Li x In, and LiInS 2 to stabilize the Li/Li 6 PS 5 Cl interface by constructing built-in electric fields, thereby enabling long-life all-solid-state lithium batteries. The work function difference between Li 2 S and Li x In generates built-in electric fields at the heterointerface, which traps the interfacial electrons and restricts their transfer to Li 6 PS 5 Cl, thereby suppressing the interfacial side reactions. Simultaneously, the built-in electric fields promote Li + adsorption and diffusion inhibiting lithium dendrite growth. Li symmetrical cells display high critical current density over 4 mA cm −2 and Li plating/stripping stability over 2000 h at 1 mA cm −2 . The assembled full cells with LiCoO 2 and LiNi 0.8 Co 0.1 Mn 0.1 (NCM811) demonstrate high capacity retention of 93% over 2000 cycles at 1 C and 87.7% over 1000 cycles at 1 C, respectively. Moreover, Li-In-S|Li 6 PS 5 Cl|NCM811 full cell shows rate capability up to 4 C. This work offers useful insights into the design of stable interfaces in all-solid-state batteries.
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产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2024
·Vol. 17
·期 24
·e202400840
·
IF 7.5
Ruojian Ma,Yaning Liu,Ruyi Fang,Jun Zhang,Ya-Hui Wang,Hui Huang,Yongping Gan,Xinping He,Xinhui Xia,Wenkui Zhang,Yang Xia,Sen Xin
Unfavorable parasitic reactions between the Ni-rich layered oxide cathode and the sulfide solid electrolyte have plagued the realization of all-solid-state rechargeable Li batteries. The accumulation of inactive by-products (P 2 S x , S, PO x n − and SO x n − ) at the cathode-sulfide interface impedes fast Li-ion transfer, which accounts for sluggish reaction kinetics and significant loss of cathode capacity. Herein, we proposed an easily scalable approach to stabilize the cathode electrochemistry via coating the cathode particles by a uniform, Li + -conductive plastic-crystal electrolyte nanolayer on their surface. The electrolyte, which simply consists of succinonitrile and Li bis(trifluoromethanesulphonyl)imide, serves as an interfacial buffer to effectively suppress the adverse phase transition in highly delithiated cathode materials, and the loss of lattice oxygen and generation of inactive oxygenated by-products at the cathode-sulfide interface. Consequently, an all-solid-state rechargeable Li battery with the modified cathode delivers high specific capacities of 168 mAh g −1 at 0.1 C and a high capacity retention >80 % after 100 cycles. Our work sheds new light on rational design of electrode-electrolyte interface for the next-generation high-energy batteries. Graphical A uniform plastic-crystal electrolyte nanolayer is coated onto the surface of Ni-rich oxide cathode particles and serves as a buffer to effectively suppress the adverse phase transition, loss of lattice oxygen and interfacial parasitic reactions with a sulfide solid electrolyte at highly delithiated cathode, which contributes improved electrochemical performance of an all-solid-stare rechargeable Li battery.
研究领域:
材料科学
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电化学
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能源存储
·
固体离子学
·
电池技术
✓ 已验证
DOI
高影响因子
Chinese Physics B
·
2022
·Vol. 31
·期 9
·098203
·
IF 1.652
Jieru Xu,Qiuchen Wang,Wenlin Yan,Liquan Chen,Hong Li,Fan Wu
Sulfide solid electrolytes are widely regarded as one of the most promising technical routes to realize all-solid-state batteries (ASSBs) due to their high ionic conductivity and favorable deformability. However, the relatively high price of the crucial starting material, Li2S, results in high costs of sulfide solid electrolytes, limiting their practical application in ASSBs. To solve this problem, we develop a new synthesis route of Li2S via liquid-phase synthesis method, employing lithium and biphenyl in 1, 2-dimethoxyethane (DME) ether solvent to form a lithium solution as the lithium precursor. Because of the comparatively strong reducibility of the lithium solution, its reaction with sulfur proceeds effectively even at room temperature. This new synthesis route of Li2S starts with cheap precursors of lithium, sulfur, biphenyl and DME solvent, and the only remaining byproduct (DME solution of biphenyl) after the collection of Li2S product can be recycled and reused. Besides, the reaction can proceed effectively at room temperature with mild condition, reducing energy cost to a great extent. The as-synthesized Li2S owns uniform and extremely small particle size, proved to be feasible in synthesizing sulfide solid electrolytes (such as the solid-state synthesis of Li6PS5Cl). Spontaneously, this lithium solution can be directly employed in the synthesis of Li3PS4 solid electrolytes via liquid-phase synthesis method, in which the centrifugation and heat treatment processes of Li2S are not necessary, providing simplified production process. The as-synthesized Li3PS4 exhibits typical Li+ conductivity of 1.85×10−4 S⋅cm−1 at 30 °C.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Nature Energy
·
2023
·Vol. 8
·期 8
·800-813
·
IF 56.7
Yan Wenlin,Mu Zhenliang,Wang Zhixuan,Huang Yuli,Wu Dengxu,Lu Pushun,Lu Jiaze,Xu Jieru,Wu Yujing,Ma Tenghuan,Yang Ming,Zhu Xiang,Xia Yu,Shi Shaochen,Chen Liquan,Li Hong,Wu Fan
All-solid-state batteries (ASSBs) with Li metal anodes or Si anodes are promising candidates to achieve high energy density and improved safety, but they suffer from undesirable lithium dendrite growth or huge volume expansion, respectively. Here we synthesize a hard-carbon-stabilized Li–Si alloy anode in which sintering of Si leads to the transformation of micro-metre particles into dense continuum. A 3D ionic-electronic-conductive network composed of plastically deformable Li-rich phases (Li 15 Si 4 and LiC 6 ) that enlarges active area and relieves stress concentration is created in the anode, leading to improved electrode kinetics and mechanical stability. With the hard-carbon-stabilized Li-Si anode, full cells using LiCoO 2 or LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes and Li 6 PS 5 Cl electrolyte achieve favourable rate capability and cycle stability. In particular, the ASSB with LiNi 0.8 Co 0.1 Mn 0.1 O 2 at high loading of 5.86 mAh cm −2 delivers 5,000 cycles at 1 C (5.86 mA cm −2 ), demonstrating the potential of using hard-carbon-stabilized Li–Si alloy anodes for practical applications of ASSBs.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）