中国物理B ›› 2024, Vol. 33 ›› Issue (8): 88201-088201.doi: 10.1088/1674-1056/ad5276

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Interface and mechanical degradation mechanisms of the silicon anode in sulfide-based solid-state batteries at high temperatures

Qiuchen Wang(王秋辰)1,2, Yuli Huang(黄昱力)1,2, Jing Xu(许晶)1,2, Xiqian Yu(禹习谦)1,2,3,†, Hong Li(李泓)1,2,3,‡, and Liquan Chen(陈立泉)1,2,3   

  1. 1 Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
    2 University of Chinese Academy of Sciences, Beijing 100049, China;
    3 Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing 101408, China
  • 收稿日期:2024-05-09 修回日期:2024-05-30 出版日期:2024-08-15 发布日期:2024-07-23
  • 通讯作者: Xiqian Yu, Hong Li E-mail:xyu@iphy.ac.cn;hli@iphy.ac.cn
  • 基金资助:
    Project supported by the Major Program of the National Natural Science Foundation of China (Grant No. 22393904), the National Key Research and Development Program of China (Grant No. 2022YFB2502200), Beijing Municipal Science & Technology Commission (Grant No. Z221100006722015), and the New Energy Vehicle Power Battery Life Cycle Testing and Verification Public Service Platform Project (Grant No. 2022-235-224).

Interface and mechanical degradation mechanisms of the silicon anode in sulfide-based solid-state batteries at high temperatures

Qiuchen Wang(王秋辰)1,2, Yuli Huang(黄昱力)1,2, Jing Xu(许晶)1,2, Xiqian Yu(禹习谦)1,2,3,†, Hong Li(李泓)1,2,3,‡, and Liquan Chen(陈立泉)1,2,3   

  1. 1 Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China;
    2 University of Chinese Academy of Sciences, Beijing 100049, China;
    3 Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing 101408, China
  • Received:2024-05-09 Revised:2024-05-30 Online:2024-08-15 Published:2024-07-23
  • Contact: Xiqian Yu, Hong Li E-mail:xyu@iphy.ac.cn;hli@iphy.ac.cn
  • Supported by:
    Project supported by the Major Program of the National Natural Science Foundation of China (Grant No. 22393904), the National Key Research and Development Program of China (Grant No. 2022YFB2502200), Beijing Municipal Science & Technology Commission (Grant No. Z221100006722015), and the New Energy Vehicle Power Battery Life Cycle Testing and Verification Public Service Platform Project (Grant No. 2022-235-224).

摘要: Silicon (Si) is a competitive anode material owing to its high theoretical capacity and low electrochemical potential. Recently, the prospect of Si anodes in solid-state batteries (SSBs) has been proposed due to less solid electrolyte interphase (SEI) formation and particle pulverization. However, major challenges arise for Si anodes in SSBs at elevated temperatures. In this work, the failure mechanisms of Si-Li$_{6}$PS$_{5}$Cl (LPSC) composite anodes above 80 $^\circ$C are thoroughly investigated from the perspectives of interface stability and (electro)chemo-mechanical effect. The chemistry and growth kinetics of Li$_{x}$Si$|$LPSC interphase are demonstrated by combining electrochemical, chemical and computational characterizations. Si and/or Si-P compound formed at Li$_{x}$Si$|$LPSC interface prove to be detrimental to interface stability at high temperatures. On the other hand, excessive volume expansion and local stress caused by Si lithiation at high temperatures damage the mechanical structure of Si-LPSC composite anodes. This work elucidates the behavior and failure mechanisms of Si-based anodes in SSBs at high temperatures and provides insights into upgrading Si-based anodes for application in SSBs.

关键词: sulfide electrolytes, silicon anodes, interface stability, degradation kinetics, all-solid-state batteries

Abstract: Silicon (Si) is a competitive anode material owing to its high theoretical capacity and low electrochemical potential. Recently, the prospect of Si anodes in solid-state batteries (SSBs) has been proposed due to less solid electrolyte interphase (SEI) formation and particle pulverization. However, major challenges arise for Si anodes in SSBs at elevated temperatures. In this work, the failure mechanisms of Si-Li$_{6}$PS$_{5}$Cl (LPSC) composite anodes above 80 $^\circ$C are thoroughly investigated from the perspectives of interface stability and (electro)chemo-mechanical effect. The chemistry and growth kinetics of Li$_{x}$Si$|$LPSC interphase are demonstrated by combining electrochemical, chemical and computational characterizations. Si and/or Si-P compound formed at Li$_{x}$Si$|$LPSC interface prove to be detrimental to interface stability at high temperatures. On the other hand, excessive volume expansion and local stress caused by Si lithiation at high temperatures damage the mechanical structure of Si-LPSC composite anodes. This work elucidates the behavior and failure mechanisms of Si-based anodes in SSBs at high temperatures and provides insights into upgrading Si-based anodes for application in SSBs.

Key words: sulfide electrolytes, silicon anodes, interface stability, degradation kinetics, all-solid-state batteries

中图分类号:  (Lithium-ion batteries)

  • 82.47.Aa
82.33.Pt (Solid state chemistry) 82.20.-w (Chemical kinetics and dynamics) 82.65.+r (Surface and interface chemistry; heterogeneous catalysis at surfaces)