Small
·
2021
·Vol. 17
·期 37
·2101326
·
IF 13.281
Chao Zheng,Jun Zhang,Yang Xia,Hui Huang,Yongping Gan,Chu Liang,Xinping He,Xinyong Tao,Wenkui Zhang
Argyrodite Li 6 PS 5 Cl with high Li + conductivity is a promising material for solid-state electrolytes (SSEs) in all-solid-state lithium batteries (ASSLBs). However, the narrow electrochemical window of Li 6 PS 5 Cl limits its applications in ASSLBs with high energy densities, and those that consist of high-voltage cathode materials and metallic lithium anodes. Unstable lithium deposition and stripping at interfaces is also a factor that restricts its industrialization. Herein, the authors investigated the electrochemical stability of Li 6 PS 5 Cl using it as both the cathode and electrolyte. The Li 6 PS 5 Cl-C/Li 6 PS 5 Cl/Li cell and symmetric Li/Li 6 PS 5 Cl/Li cells failed after a certain number of cycles, and subsequently healed electrochemically. This failure/healing phenomenon recurred during the cycling process. The self-healing behavior is closely related to the electrochemical window, which suggests that it can be controlled by the charge–discharge voltage range. In-depth X-ray photoelectron spectroscopy, in situ Raman spectroscopy, and in situ electrochemical impedance spectroscopy revealed the reversible Li 6 PS 5 Cl decomposition and metallic lithium growth inside the electrolyte during the cycling process. This self-healing behavior is mainly attributed to the reciprocating lithium growth and reversible redox reaction of the Li 6 PS 5 Cl decomposition. The proposed self-healing mechanism is a key aspect for sulfide-based SSEs, guiding the interface modification, and material design of ASSLBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 39
·19231-19240
·
IF 9.931
Minjie Xuan,Weidong Xiao,Hongjie Xu,Yonglong Shen,Zhenzhen Li,Shijie Zhang,Zhuo Wang,Guosheng Shao
The development of a solid electrolyte with superb Li+ conductivity is the key to enabling safe and high-performance all-solid lithium ion batteries which are free of the safety issues associated with flammable organic liquid electrolyte. Systematic experimental work has been carried out as a follow up to our recent theoretical prediction that superb ionic conductivity could be achieved through the tuning of the lattice chemistry in the cubic argyrodite Li6PS5Cl. Remarkable enhancement of the ionic conductivity has been achieved through the combined effect of excess Li and substitution of S with Te. This leads to an alloy, Li6.25PTe0.125S5.125Cl0.75, having the superb Li+ conductivity of 4.5 mS cm−1 at 25 °C, together with a low activation energy of 0.16 eV to safeguard adequate ionic conductivity at low temperature. This current work conclusively affirms the theoretical outcome that the superb ionic conductivity is attributed to weakened bonding, an enlarged unit cell, and a softened lattice, making it easier for the long-distance diffusion of Li+. In addition, this new class of solid electrolyte based on cubic chalcogenide is electrochemically compatible with the Li anode over a large potential window up to 7 V, which is highly desirable for high performance solid lithium ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
固体离子学
·
无机化学
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
·Vol. 27
·期 6
·3455-3462
·
IF 2.9
Yuanyuan Lin,Hanzhou Liu,Yaqi Hu,Yang Lu,Zongliang Zhang,Yang Liu,Yongle Chen,Kun Zhang,Shuo Yin,Fangyang Liu
The practical applications of all-solid-state batteries (ASSBs) are hindered by poor Li kinetics in electrodes due to the inadequate contact between the cathode active materials (CAMs) and solid-state electrolytes (SSEs). Therefore, improving the contact interface between CAMs and SSEs is necessary to improve the cathodic Li kinetics by increasing the lithium-ion transport sites. To address this issue, sub-micrometer Li6PS5Cl (SU-LPSC) particles of high specific areas were utilized to fabricate cathodes with high mass loading. SU-LPSC powders can provide fruitful ionic transport pathways by suppressing inert voids in the electrodes, forming conformal contacts. The reduced porosity contributed to the decrease of the ion tortuosity from 3.91 to 1.77. Therefore, the apparent lithium-ion diffusion coefficient improved by nearly 65%. The SU-LPSC-based cathode/LPSC/Li-In battery exhibits good capacity and cycle performance with different cathode loading amounts. Those assembled batteries utilizing SU-LPSC cathode deliver comparable initial discharge capacities of 197.5 mA h g−1 and an initial coulombic efficiency of 82.4% when cycled at 0.1C, and maintain 93.4% at 0.5C after 200 cycles at room temperature. In comparison to the IN-LPSC cathode battery, the capacity retention after 200 cycles is enhanced by 8.7%. This study investigated the sub-micrometer particle sizes of SSEs to determine the Li kinetics in the cathode, reflecting the good performance of ASSBs, providing a valuable reference for designing high-energy cathodes and optimizing composite cathode structures.
研究领域:
材料科学
·
电化学
·
储能技术
·
固体离子学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
·
2022
·Vol. 13
·期 5
·2202756
·
IF 29.698
Yaqi Hu,Zhen Sun,Zongliang Zhang,Siliang Liu,Fangbo He,Yang Liu,Zhi Zhuang,Fangyang Liu
Outstanding interfacial issues exist between oxide cathodes and sulfide electrolytes in all-solid-state lithium batteries (ASSLBs), while high-capacity Li-rich sulfide cathodes are gaining attention for application. Herein, a sulfide cathode active material Li 2 TiS 3 (LTS) that is chemically compatible with sulfide solid electrolytes, is used in high-performance Li 6 PS 5 Cl-based ASSLBs at room temperature. The batteries demonstrate a maximum discharge capacity of 423.2 mAh g −1 (910 Wh kg −1 based on Li 2 TiS 3 ) with 95% capacity retention after 100 cycles at 0.1 C (0.33 mA cm −2 ). Traces of elemental sulfur on the surface of LTS are mainly responsible for the excessive Li-intercalation and the capacity exceedance. The Li 6 PS 5 Cl is also found to offer a nonnegligible capacity (at least 27% of excess capacity) by comparing the Li 6 PS 5 Cl-based and Li 3 YCl 6 -based cells using Li 2 TiS 3 as cathode active material. During long cycling, the amorphization and degradation of Li 2 TiS 3 and Li 6 PS 5 Cl cause capacity decay. The electrochemical kinetics of Li 6 PS 5 Cl-based cells are evaluated as a reference to further exploit the potential of Li 2 TiS 3 material for practical applications in ASSLBs. Overall, this superior Li-rich sulfide material is an attractive alternative to oxide cathodes for the development of high-performance ASSLBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2019
·Vol. 10
·期 4
·1903311
·
IF 24.884
Jun Zhang,Chao Zheng,Lujie Li,Yang Xia,Hui Huang,Yongping Gan,Chu Liang,Xinping He,Xinyong Tao,Wenkui Zhang
High-performance rechargeable all-solid-state lithium metal batteries with high energy density and enhanced safety are attractive for applications like portable electronic devices and electric vehicles. Among the various solid electrolytes, argyrodite Li 6 PS 5 Cl with high ionic conductivity and easy processability is of great interest. However, the low interface compatibility between sulfide solid electrolytes and high capacity cathodes like nickel-rich layered oxides requires many thorny issues to be resolved, such as the space charge layer (SCL) and interfacial reactions. In this work, in situ electrochemical impedance spectroscopy and in situ Raman spectroscopy measurements are performed to monitor the detailed interface evolutions in a LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM)/Li 6 PS 5 Cl/Li cell. Combining with ex situ characterizations including scanning electron microscopy and X-ray photoelectron spectroscopy, the evolution of the SCL and the chemical bond vibration at NCM/Li 6 PS 5 Cl interface during the early cycles is elaborated. It is found that the Li + ion migration, which varies with the potential change, is a very significant cause of these interface behaviors. For the long-term cycling, the SCL, interfacial reactions, lithium dendrites, and chemo-mechanical failure have an integrated effect on interfaces, further deteriorating the interfacial structure and electrochemical performance. This research provides a new insight on intra and intercycle interfacial evolution of solid-state batteries.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源存储
·
界面化学
·
电池技术
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 40
·2312305
·
IF 27.4
Shenghao Jing,Yang Lu,Yuting Huang,Hanzhou Liu,YuXing Shen,Wuqi Kuang,Huaqing Shen,Siliang Liu,Zongliang Zhang,Fangyang Liu
The silicon-based anodes are one of the promising anodes to achieve the high energy density of all-solid-state batteries (ASSBs). Nano silicon (nSi) is considered as a suitable anode material for assembling sheet-type sulfide ASSBs using thin free-standing Li 6 PS 5 Cl (LPSC) membrane without causing short circuit. However, nSi anodes face a significant challenge in terms of rapid capacity degradation during cycling. To address this issue, dual-function Li 4.4 Si modified nSi anode sheets are developed, in which Li 4.4 Si serves a dual role by not only providing additional Li + but also stabilizing the anode structure with its low Young's modulus upon cycling. Sheet-type ASSBs equipped with the Li 4.4 Si modified nSi anode, thin LPSC membrane, and LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) cathode demonstrate exceptional cycle stability, with a capacity retention of 96.16% at 0.5 C (1.18 mA cm −2 ) after 100 cycles and maintain stability for 400 cycles. Furthermore, a remarkable cell-level energy density of 303.9 Wh kg −1 is achieved at a high loading of 5.22 mAh cm −2 , representing a leading level of sulfide ASSBs using electrolyte membranes at room temperature. Consequently, the chemically stable slurry process implemented in the fabrication of Li 4.4 Si-modified nSi anode sheet paves the way for scalable applications of high-performance sulfide ASSBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Materiomics
·
2019
·Vol. 6
·期 1
·70-76
·
IF 0
Shuo Wang,Xue Zhang,Sijie Liu,Chengzhou Xin,Chuanjiao Xue,Felix Richter,Liangliang Li,Lizhen Fan,Yuanhua Lin,Yang Shen,Jürgen Janek,Ce-Wen Nan
Bulk-type all-solid-state batteries (ASSBs) using sulfide solid electrolyte are considered as a promising alternative to commercial lithium-ion batteries owing to their high energy density and safety. However, cell energy density is often comparatively low due to use of a thick solid electrolyte separator and a lithium alloy as anode. For achieving high-performance ASSBs, creating a thin free-standing electrolyte with high-conductivity and good cycling stability against lithium anode is essential. In this work, we present Li 6 PS 5 Cl/poly(vinylidene difluoride) (LPSCl/PVDF) composite electrolytes prepared by a slurry method. The influence of the PVDF content on the microstructure, morphology, ionic conductivity and activation energy of the LPSCl/PVDF electrolytes is systematically investigated. Free-standing LPSCl/PVDF membranes with a thickness of 100–120 μm and a high ionic conductivity of about 1·10 −3 S cm −1 at 25 °C are obtained. After adding PVDF to the LPSCl electrolyte, the cycling stability of the LPSCl electrolyte against lithium metal improves significantly. Therefore, LPSCl/PVDF composite electrolytes are promising candidates to be used in ASSBs.
研究领域:
材料科学
·
储能
·
电化学
·
锂离子电池
✓ 已验证
DOI
Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-17
·
IF 36.3
Gao Xin,Chen Ya,Zhen Zheng,Cui Lifeng,Huang Ling,Chen Xiao,Chen Jiayi,Chen Xiaodong,Lee Duu-Jong,Wang Guoxiu
This work provides a brand-new approach to the “conversion-protection” strategy to overcome the drawbacks of composite cathode interfaces.
The Mo 3 Ni 3 N not only makes it difficult for hydroxide groups (-OH) to survive on the surface but also allows the in situ surface reconstruction to generate the ultra-stable MoS 2 -Mo 3 Ni 3 N heterostructures after the initial cycling stage.
The Mo-Ni@NPCs/LCO/LPSC-based ASSLBs achieve high-capacity retention (90.62%) and excellent cycle life (1000 cycles).
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Energy Research
·
2021
·
IF 4.008
Chao Zheng,Kai Wang,Lujie Li,Hui Huang,Chu Liang,Yongping Gan,Xinping He,Wenkui Zhang,Jun Zhang
Among many lithium secondary batteries, lithium–sulfur batteries stand out because of their high theoretical specific energy, low cost, non-toxicity and the fact that they cause no environmental pollution. However, due to poor electronic and ionic conductivity, shuttle effect, lithium dendrites and other defects, it remains a big challenge to achieve large-scale application of lithium-sulfur batteries. Here we report an all-solid-state lithium–sulfur battery based on Li-argyrodite Li6PS5Cl solid-state electrolytes through a slurry-coating method. Li6PS5Cl with a high ionic conductivity of 1.3 × 10–3 S cm−1 at room temperature is used as the solid electrolyte and the ion conductive additive in the electrode. The sulfur-based composite cathode is fabricated through a slurry-coating process by dispersing sulfur, Li6PS5Cl, ethyl cellulose, and carbon black in 1,3-dioxolane (DOL). This method can disperse the Li6PS5Cl around sulfur particles well, and the solvent does not react with any component of composite cathodes during preparation. The battery delivers a high discharge capacity of 962 mA h g−1 at room temperature for the first cycle at 80 mA g−1. While the Coulombic efficiency is approximately 99.5% during 100 cycles. This work provides a new insight into the combination method between the sulfide-type SSEs and sulfur cathodes, which is critical to the electrochemical performance of all-solid-state lithium-sulfur batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
纳米材料
·
界面化学
·
电极工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Zhigao Luo,Xianyou Wang
Composite polymer electrolytes (CPEs), which are made up of sulfide solid electrolyte Li 6 PS 5 Cl dispersed in solid polymer electrolytes (SPEs) based on the poly (ethylene oxide) (PEO), has been prepared by adopting solution casting method. The results show that the addition of appropriate amount of Li 6 PS 5 Cl can enhance lithium-ion conductivity and interfacial stability of solid polymer electrolyte, which can play an active role in the electrochemical properties of the improving all-solid-state LiFePO 4 /Li batteries. Especially, the PEO-1 wt% Li 6 PS 5 Cl exhibits a high lithium-ion conductivity of 8.84 × 10 −4 S/cm at 80 ℃ and 7.58 × 10 −5 S/cm at 30 ℃. Compared with the SPE, the PEO-1 wt% Li 6 PS 5 Cl has smaller interfacial impedance and more stable interface with lithium metal. Therefore, all-solid-state LiFePO 4 /Li batteries assembled by the PEO-1 wt% Li 6 PS 5 Cl represent higher coulomb efficiency, and better cycle stability with high initial discharge capacity of 155.43 mAh/g, 134.95 mAh/g at current rates of 0.2C, 0.5C at 60 ℃, respectively.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子化学
·
固态离子学
✓ 已验证
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Ailing Hwang,Yulin Ma,Yi Cao,Qin Li,Long Wang,Xinqun Cheng,Pengjian Zuo,Chunyu Du,Yunzhi Gao,Geping Yin
Li 6 PS 5 Cl-coated Li 4 Ti 5 O 12 materials was fabricated by a simple liquid-phase treatment method. Charge-discharge tests show that Li 6 PS 5 Cl-coated Li 4 Ti 5 O 12 (LTO@LPSCl)/Li 6 PS 5 Cl/Li all-solid-state lithium batteries exhibit high reversible capacity (~158 mA h·g -1 ) after 250 cycles under 0.05 C and excellent rate capacity (~50 mA h·g -1 ) under 1 C at 80 °C .A combination of scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDX) mapping, and electrochemical impedance spectra (EIS) reveals that good wettability of liquid with Li 4 Ti 5 O 12 materials and Li 6 PS 5 Cl is responsible for Li 6 PS 5 Cl nanoparticle coated on the surface of Li 4 Ti 5 O 12 materials homogenously, which build the stable interface between active materials and solid state electrolyte, reduce the interface resistance effectively, and result in excellent electrochemical performances.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源存储
·
纳米材料
✓ 已验证
DOI
高影响因子
Energy & Environmental Materials
·
2023
·
IF 15
Junwu Sang,Bin Tang,Yong Qiu,Yongzheng Fang,Kecheng Pan,Zhen Zhou
All-solid-state lithium metal batteries (ASSLMBs) with solid electrolytes (SEs) have emerged as a promising alternative to liquid electrolyte-based Li-ion batteries due to their higher energy density and safety. However, since ASSLMBs lack the wetting properties of liquid electrolytes, they require stacking pressure to prevent contact loss between electrodes and SEs. Though previous studies showed that stacking pressure could impact certain performance aspects, a comprehensive investigation into the effects of stacking pressure has not been conducted. To address this gap, we utilized the Li 6 PS 5 Cl solid electrolyte as a reference and investigated the effects of stacking pressures on the performance of SEs and ASSLMBs. We also developed models to explain the underlying origin of these effects and predict battery performance, such as ionic conductivity and critical current density. Our results demonstrated that an appropriate stacking pressure is necessary to achieve optimal performance, and each step of applying pressure requires a specific pressure value. These findings can help explain discrepancies in the literature and provide guidance to establish standardized testing conditions and reporting benchmarks for ASSLMBs. Overall, this study contributes to the understanding of the impact of stacking pressure on the performance of ASSLMBs and highlights the importance of careful pressure optimization for optimal battery performance.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）