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

作　　者：王秋辰 黄昱力 许晶 禹习谦 李泓 陈立泉 Qiuchen Wang;Yuli Huang;Jing Xu;Xiqian Yu;Hong Li;Liquan Chen(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;University of Chinese Academy of Sciences,Beijing 100049,China;Huairou Division,Institute of Physics,Chinese Academy of Sciences,Beijing 101408,China)

机构地区：[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

出　　处：《Chinese Physics B》2024年第8期117-126,共10页中国物理B（英文版）

基　　金：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);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℃are thoroughly investigated from the perspectives of interface stability and(electro)chemo-mechanical effect.The chemistry and growth kinetics of Lix Si|LPSC interphase are demonstrated by combining electrochemical,chemical and computational characterizations.Si and/or Si–P compound formed at Lix 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 

分 类 号：TM912[电气工程—电力电子与电力传动]