ACS Applied Energy Materials
·
2023
·
IF 6.4
Changfei Zou,Zihao Zang,Xiyuan Tao,Lingguang Yi,Xiaoyi Chen,Xiaoyan Zhang,Li Yang,Xianhu Liu,Xianyou Wang
All-solid-state lithium batteries (ASSLBs) composed of sulfide-based solid-state electrolyte and LiNixMnyCo1–x–yO2 (NMC) cathode are expected to become the promising next generation of energy storage systems due to their great potential in highly improved safety and energy density. However, the poor interfacial stability between the NMC cathode and sulfide-based electrolyte remains an important challenge for the commercialization of ASSLBs. In this study, a thin layer of fast lithium-ion conductor Li1.3Al0.3Ti1.7(PO4)3 (LATP) with a thickness of 8 nm was coated at the interface between LiNi0.8Co0.1Mn0.1O2 (NCM811) and Li5.5PS4.5Cl1.5 via a facile wet chemical method to improve interfacial stability. It has been found that the nanoscale LATP coating layer can not only accelerate lithium ions across the NCM811/Li5.5PS4.5Cl1.5 interface but also effectively alleviate the interfacial problems. The initial discharge capacity of the as-prepared LATP@NCM811/Li5.5PS4.5Cl1.5/Li batteries at 0.1 C is 151.5 mAh/g, and the capacity retention rate is 81.6% after 100 cycles at room temperature. The results indicate that interfacial modification with the nanosized LATP coating is an effective strategy for providing more possibilities for commercial application of ASSLBs.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
Journal of Materiomics
·
2025
·
IF 9.6
Zhixing Wan,Shuo Wang,Yahao Mu,Ruihua Zhou,Hang Liu,Tingwu Jin,Di Wu,Jianlong Xia,Ce-Wen Nan
Organic cathode materials have garnered significant attention for their potential application in lithium-ion batteries due to their lightweight nature, tunable structures, high energy density, and environmental friendliness. However, the dissolution of organic cathodes in liquid electrolytes often leads to poor cycling stability, which limits their practical application. In this study, a composite cathode was prepared by ball milling the PTCDA/CuS (perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) with a sulfide-based electrolyte and carbon nanotubes. By optimizing the component ratios, the assembled all-solid-state batteries (ASSBs) show a high discharge capacity of 210 mA⸱h/g after 200 cycles without any capacity degradation at a current density of 33.0 mA/g. Through comprehensive characterization techniques including X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), the coordination of Cu 2+ and the formation of sulfur-linked polymers during the charge-discharge processes are elucidated, and the reversibility of the electrochemical reactions has been confirmed. This work highlights the excellent compatibility between organic cathodes and sulfide-based electrolytes, providing a new way for the development of high-performance ASSBs with high energy density and extended lifespan.
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
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 32
·2100921
·
IF 30.849
Pushun Lu,Lilu Liu,Shuo Wang,Jieru Xu,Jian Peng,Wenlin Yan,Qiuchen Wang,Hong Li,Liquan Chen,Fan Wu
Sulfide solid electrolytes (SEs) are recognized as one of the most promising candidates for all-solid-state batteries (ASSBs), due to their superior ionic conductivity and remarkable ductility. However, poor air stability, complex synthesis process, low yield, and high production cost obstruct the large-scale application of sulfide SEs. Herein, a one-step gas-phase synthesis method for sulfide SEs with oxide raw materials in ambient air, completely getting rid of the glovebox and thus making large-scale production possible, is reported. By adjusting substituted elements and concentrations, the ionic conductivity of Li 4- x Sn 1- x M x S 4 can reach 2.45 mS cm −1 , which represents the highest value among all reported moist-air-stable and recoverable lithium-ion sulfide SEs reported. Furthermore, ASSBs with air/water-exposed and moderate-temperature-treated Li 3.875 Sn 0.875 As 0.125 S 4 even maintains superior performances with the highest reversible capacity (188.4 mAh g −1 ) and the longest cycle life (210 cycles), which also breaks the record. Therefore, it may become one of the most critical breakthroughs during the development of sulfide ASSBs toward its practical application and commercialization.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhao Jiang,Zhongxu Li,Xiuli Wang,Changdong Gu,Xinhui Xia,Jiangping Tu
All-solid-state lithium-metal batteries (ASSLMBs) with sulfide electrolytes have attracted attention owing to their superior safety and high energy density. However, interfacial instability of sulfide electrolytes against Li metal still hinders their applications. Herein, F-doping is adopted to optimize the structure of Li10SnP2S12. It is demonstrated that the Li9.95SnP2S11.95F0.05 (LSPSF) electrolyte exhibits a high ionic conductivity of 6.4 mS cm–1 because of F-doping, which can reduce the impurity Li2SnS3 and generate Li+ vacancies. In addition, the Li6PS5I (LPSI) glass–ceramic interlayer is employed to enhance the interfacial stability between the sulfide electrolyte and Li metal by restraining the reduction of Sn4+ cations, as indicated by X-ray photoelectron spectroscopy (XPS). As a result, the assembled ASSLMBs with the LPSI interlayer deliver high initial discharge capacity and remarkable cycling stability. This work provides a new design route for manufacturing high-performance ASSLMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Jie Shi,Ping Li,Kun Han,Dong Sun,Wang Zhao,Zhiwei Liu,Gemeng Liang,Kenneth Davey,Zaiping Guo,Xuanhui Qu
Sulfide electrolytes (SEs)-based all-solid-state lithium batteries (ASSLBs) are advantageous over traditional lithium-ion batteries (LIBs) because of high energy density and safety. Unfortunately, the commercialization of SEs-based ASSLBs is presently hindered by interfacial instability between SEs and active materials, sluggish dynamics and poor cycling performance. Here we report, for the first time, a stable and conductive Li 2 O buffering coating for Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) in ASSLBs using SEs of Li 6 PS 5 Cl via a facile one-step sintering. We show using judiciously combined computation and experiment that Li 2 O buffering improves the stability of NCM811 and significantly boosts transfer of Li + . Via tuning the thickness of the Li 2 O buffer, we demonstrate the high initial discharge capacity of 189.66 mAh g − 1 (0.1C) and rate capability of 61.71 mAh g − 1 (3C), together with outstanding long-term cycling performance of ∼ 2600 cycles at 1C with capacity retention of 81.47%, and Coulombic efficiency of 99.9%. We conclude that conductive Li 2 O buffering can be used to obviate interfacial instability between SEs and active materials and to boost dynamics and cycling performance. Findings will be of immediate benefit to a range of researchers in design for high-performance ASSLBs for practical application and commercialization.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2013
·Vol. 17
·期 11
·2909-2915
·
IF 2.279
Zhang Jing Bo,Zhao Fei Yan,Tang Guang Shi,Lin Yuan
PbS electrode with high catalytic activity to S n
2− reduction certificated by the measurements of electrochemical impedance spectroscopy and cyclic voltammetry was prepared by a simple method. The high catalytic activity makes it be a low-cost alternative counter electrode to platinum (Pt) to be used in quantum dots-sensitized solar cells (QDSSCs) based on polysulfide electrolyte. The photovoltaic performance enhancement of the quantum dots (QDs)-sensitized semiconductor thin films due to the PbS counter electrode was evaluated by fabricating QDSSCs based on CdSe QDs-sensitized ZnO (SnO 2 ) thin film. CdSe QDs-sensitized ZnO thin film has the lower internal total series resistance and electron transmission time, the higher electron lifetime and electron collection efficiency than the CdSe QDs-sensitized SnO 2 thin film. Replacing the Pt counter electrode with the PbS counter electrode leads to more improvement on the short circuit photocurrent density for QDSSC based on the ZnO thin film than the SnO 2 thin film. Therefore, the process to limit the photovoltaic performance of CdSe QDs-sensitized solar cell and the possible way to improve the photovoltaic performance were analyzed.
研究领域:
材料科学
·
能源技术
·
光电化学
✓ 已验证
产品关联
DOI
高影响因子
SOLID STATE IONICS
·
2025
·
IF 3.3
Jie-Fu Zhuo,Zhi-Feng Yao
The argyrodite-type sulfide electrolytes (Li 6 PS 5 X, X = Cl, Br, I) have demonstrated numerous benefits for high-performance and secure all-solid-state lithium‑sulfur batteries (ASSLSBs). These advantages include their rapid lithium (Li) ion conduction and exceptional compatibility with the anode. Nevertheless, despite these benefits, the key obstacles for their implementation are the need for higher room-temperature ionic conductivity, improved air/moisture compatibility, and enhanced electrochemical stability. In this study, we propose a halogen-rich argyrodite (Li 5.3 PS 4.3 Cl 1.7-x Br x ) to obtain ultrafast ionic conductivity at ambient temperature. To enhance the ionic transport channel, the anion disorder on the site is optimized and the Li vacancies in the structure are increased by substituting anions with halogens (Cl/Br). The Li 5.3 PS 4.3 Cl 0.85 Br 0.85 is synthesized effectively by a high-energy ball milling process, resulting in a remarkable ionic conductivity of 9.07 mS⋅cm −1 at room temperature. In addition, a SiO 2 dopant is utilized to strengthen the lattice structure of the solid-state electrolyte (Li 5.3+y Si y P 1-y S 4.3-2y O 2y Cl 0.85 Br 0.85 ) in order to improve its resistance to air/moisture and enhance its electrochemical stability within specific voltage ranges. The Li 5.4 Si 0.1 P 0.9 S 4.1 O 0.2 Cl 0.85 Br 0.85 with optimized composition demonstrates an ionic conductivity of 8.2 mS⋅cm −1 at room temperature and exceptional stability in air. The ASSLSBs containing Li 5.4 Si 0.1 P 0.9 S 4.1 O 0.2 Cl 0.85 Br 0.85 exhibit impressive specific capacities of 1191 mAh⋅g −1 (0.1C after the initial cycle) and 989 mAh⋅g −1 (0.1C after 100 cycles) at room temperature. Additionally, they demonstrate significant cyclability (83.04 % after 100 cycles) and excellent Coulombic efficiency (>99.5 %). This study presents a novel strategy to promote the application of sulfide electrolytes in fabricating ASSLSBs.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chenxi Gao,Xiao Xu,Tiansheng Bai,Jun Cheng,Zhen Zeng,Hongqiang Zhang,Naixuan Ci,Wei Zhai,Qing Ma,Jingyu Lu,Jun Ma,Lijie Ci,Deping Li
Nickel-rich layered oxide with high reversible capacity and high working potentials is a prevailing cathode for high-energy-density all-solid-state lithium batteries (ASSLBs). However, compared to the liquid battery system, ASSLBs suffer from poor Li-ion migration kinetics, severe side reactions, and undesired formation of space charge layers, which result in restricted capacity release and limited rate capability. In this work, we reveal that the capacity loss lies in the H2–H3 phase transition period, and we propose that the inconsistent interfacial Li-ion migration is the arch-criminal. We introduce Si doping to stabilize the bulk structure and Li4SiO4 fast ionic conductor coating to regulate the interfacial behaviors between the Ni-rich cathode and sulfide-based solid electrolyte Li6PS5Cl. The modified NCM@LSO-2||LPSCl||Li–In ASSLBs deliver a high reversible capacity of 183.5 mA h g–1 at 0.1C, 30.3% higher than the bare NCM811 electrode. Besides, the interfacial regulation strategy enables the operation at a high rate of 5.0C and achieves a high capacity retention ratio of ∼85.8% after 500 cycles at 1.0C. Furthermore, the underlying mechanisms are well investigated through kinetic analyses and theoretical simulations. This work provides an in-depth understanding on the interfacial degradations between Ni-rich cathodes and sulfide-based all-solid-state electrolytes from the view of kinetic limitations and offers potential solutions.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Qiyue Luo,Siwu Li,Chaochao Wei,Zhongkai Wu,Chen Liu,Ziling Jiang,Lin Li,Shaoqing Chen,Chuang Yu
Sulfide-based all-solid-state batteries are currently a focal point of research for next-generation energy storage solutions. However, the poor antioxidative stability of sulfide electrolytes limits their practical applications. In this study, we strengthen sulfur-related bonding interactions by regulating the local charge density of the surrounding sulfur atoms, thereby enhancing the oxidative stability of sulfide electrolytes. First-principles calculations and experimental results demonstrate that substituting certain sulfur in Li9.9SnP2S11.9Br0.1 with oxygen leads to an increase in the local electronic density around unsubstituted sulfur atoms and a reduction in cation–anion bond lengths, which subsequently strengthens the bonds including P–S and Sn–S. Remarkably, the tailored electrolyte also exhibits significant improvements in air stability and chemical compatibility with halide electrolytes. Batteries constructed with the obtained Li9.9SnP2S10.9Br0.1O1.0 electrolyte demonstrated greatly enhanced electrochemical performance. Our results highlight how local charge distribution regulation enhances the chemical and electrochemical stability of sulfide electrolytes, offering valuable insights for creating high-performance all-solid-state batteries.
研究领域:
材料科学
·
能源存储
·
固体物理
✓ 已验证
产品关联
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 ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Zhikai Huang,Zhihao Yan,Dingding Zhu,Xuedong Zhang,Shuaiyu He,Jianyu Huang,Guobao Xu
Despite lithium-argyrodite electrolytes have attracted great attention due to the high ionic conductivity and relatively lower cost, their applications are hindered by the inferior air stability and poor Li compatibility. Herein, we report a Sn/I co-doping the Li 6 PS 5 Cl strategy to overcome above obstacles. The optimized LPSC-0.05SnI 4 exhibits high ionic conductivity of 3.9 × 10 −3 S cm −1 at room temperature, and improved air stability. More importantly, an in situ formed LiI-rich interface on the lithium anode is introduced through the LPSC-0.05SnI 4 . As a result, the Li/LPSC-0.05SnI 4 /Li symmetric batteries deliver high critical current density of 1.45 mA cm −2 and a remarkable steady Li plating/stripping performance over 6000 h at 0.1 mA cm −2 . The assembled LNO@NMC811/LPSC-0.05SnI 4 /Li all-solid-state batteries display prominent capacity and cycling stability. This work provides a practical and effective method for designing versatile and high-performance sulfide-based solid electrolytes .
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Qiyue Luo,Chuang Yu,Chaochao Wei,Shuai Chen,Shaoqing Chen,Ziling Jiang,Linfeng Peng,Shijie Cheng,Jia Xie
Li 10 GeP 2 S 12 shows great potential as solid electrolytes for solid-state batteries due to its ultrahigh Li-ion conductivity. However, the high cost of Ge and the poor stability limit its applications. Replacing Ge with Sn can significantly lower the cost and maintains the high conductivity, while the corresponding Li 10 SnP 2 S 12 still suffers the low interfacial stability with the bare high voltage layered oxide cathodes. Herein, Li 10 SnP 2 S 12 with high Li-ion conductivity up to 4.79 mS cm −1 has been synthesized. All-solid-state battery using the cathode consisting of bare LiNi 0.6 Co 0.2 Mn 0.2 O 2 and Li 10 SnP 2 S 12 shows low capacities and poor cyclability due to side reactions between those two particles. To improve the interfacial stability, a highly conductive Li 3 InCl 6 electrolyte is introduced both in the cathode mixture and between the cathode layer and Li 10 SnP 2 S 12 solid electrolyte layer. This new configuration delivers superior electrochemical performances at different operating temperatures. It delivers high initial discharge capacities of 176.1 mAh g −1 , 186.9 mAh g −1 , and 73.7 mAh g −1 at 0.1C when operated at room temperature, 60 o C, and −20 o C, respectively. The superior battery performances are attributed to the excellent electrochemical stability of Li 3 InCl 6 electrolyte towards bare LiNi 0.6 Co 0.2 Mn 0.2 O 2 cathode. This work provides a guideline to design Li 10 SnP 2 S 12 -based all-solid-state lithium batteries with high energy density and long span life.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）