Molding of Li5.5PS4.5Cl1.5 Particles Based on Regulating Li+ Transport for All-Solid-State Li Metal Battery.

Journal: Angewandte Chemie (International ed. in English)
Published Date: Dec 3, 2025

Abstract

All-solid-state Li metal batteries (ASSLBs) are coming with sulfide solid-state electrolytes (S-SSEs) for superior Li+ conductivity, but irregular particles and interfaces lead to disorder Li+ flux in S-SSEs that hinder pure Li as an anode. Specially, its mesoscopic structure cannot be adequately described by average size, making it difficult to analyze Li+ flux effectively. Herein, a model is constructed on the molding of Li5.5PS4.5Cl1.5 (LPSC) particles and defined size as the number (N) and consistency (σ) to evaluate their effects on Li+ transfer and concentration uniformity. Through machine learning of calculation data (Li+ concentration with N and σ) and experimental results, excessive interfaces can hinder Li+ transport and local aggregation of irregular interfaces leads to uneven ion transport. Therefore, a particle size gradient S-SSEs (induced by different size LPSC particles) is predicted to achieve fast and uniform Li+ transport. Subsequently, this designed S-SSE is applied in ASSLBs, which can complete a 1000 h cycle with capacity retention exceeding 80%. This study elucidates that the long cycle ASSLBs can be achieved by adjusting the molding of LPSC particles. Specifically, it demonstrates that the Li+ flux of the whole S-SSEs can be optimized through gradient size design.

Authors

  • Guanwu Li
    State Key Laboratory of High Pressure and Superhard Materials, and School of Materials Science and Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun, 130013, P. R. China.
  • Dong Wang
    Department of Neurosurgery, Tianjin Medical University General Hospital, Tianjin, China.
  • Bo Gao
  • Changru Rong
    General Research and Development Institute, China FAW Corporation Limited, Changchun, 130013, P. R. China.
  • Xuepeng Li
    Research Institute of Food Science, Bohai University, Jinzhou 121013, China; College of Chemistry, Chemical Engineering and Food Safety, Bohai University, Jinzhou 121013, China.
  • Zixiao Zhang
    State Key Laboratory of High Pressure and Superhard Materials, and School of Materials Science and Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun, 130013, P. R. China.
  • Jiayu Wang
    Department of Cardiology, the Second Hospital of Shandong University, 250033 Jinan, Shandong, China.
  • Jinyi Zhao
    State Key Laboratory of High Pressure and Superhard Materials, and School of Materials Science and Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun, 130013, P. R. China.
  • Xiaofei Yang
    Guizhou University, Guiyang, China Guizhou University Guiyang China.
  • Jian Wang
    Veterinary Diagnostic Center, Shanghai Animal Disease Control Center, Shanghai, China.
  • Xinyan Zhou
    Department of Medicine, Yong Loo Lin School of Medicine, National University of Singapore, Singapore.
  • Hongzhen Lin
    i-Lab & CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano-tech and Nano-bionics, Chinese Academy of Sciences, Suzhou, 215123, P. R. China.
  • Wei Zhang
    The First Affiliated Hospital of Nanchang University, Nanchang, China.
  • Yingze Song
    School of Materials and Chemistry, State Key Laboratory of Environment-Friendly Energy Materials, Southwest University of Science and Technology, Mianyang, 621010, China.
  • Zhi Chang
    School of Materials Science and Engineering, Central South University, Changsha, Hunan, 410083, China.
  • Yunfeng Jiang
    General Research and Development Institute, China FAW Corporation Limited, Changchun, 130013, P. R. China.
  • Xing Ou
    Hunan Province Key Laboratory of Chemical Power Source, School of Materials Science and Engineering, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, P. R. China.
  • Weitao Zheng
    School of Intelligent Sports Engineering, Wuhan Sports University, Wuhan, Hubei, People's Republic of China.

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