High-modulus solid electrolyte interphase layer with gradient composition enables long-cycle all-solid-state lithium-sulfur batteries  

作　　者：Huanhuan Duan Jinhai Liu Jiafeng He Linyuan Ma Yuanfu Deng Guohua Chen 

机构地区：[1]Guangdong Provincial Key Laboratory of Fuel Cell Technology,School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640,Guangdong,China [2]Guangdong Provincial Research Center of Electrochemical Energy Engineering,South China University of Technology,Guangzhou 510640,Guangdong,China [3]School of Energy and Environment,City University of Hong Kong,Tat Chee Avenue,Kowloon,Hong Kong 999077,China

出　　处：《Journal of Energy Chemistry》2024年第11期87-95,共9页能源化学（英文版）

基　　金：National Natural Science Foundation of China (Grant Nos. 22178125 and 21875071)。

摘　　要：All-solid-state lithium-sulfur batteries(ASSLSBs) have become one of the most potential candidates for the next-generation high-energy systems due to their intrinsic safety and high theoretical energy density.However, PEO-based ASSLSBs face the dilemma of insufficient Coulombic efficiency and long-term stability caused by the coupling problems of dendrite growth of anode and polysulfide shuttle of cathode. In this work, 1,3,5-trioxane(TOX) is used as a functional additive to design a PEO-based composite solidstate electrolyte(denoted as TOX-CSE), which realizes the stable long-term cycle of an ASSLSB. The results show that TOX can in-situ decompose on the anode to form a composite solid electrolyte interphase(SEI) layer with rich-organic component. It yields a high average modulus of 5.0 GPa, greatly improving the mechanical stability of the SEI layer and thus inhibiting the growth of dendrites. Also,the robust SEI layer can act as a barrier to block the side reaction between polysulfides and lithium metal.As a result, a Li-Li symmetric cell assembled with a TOX-CSE exhibits prolonged cycling stability over 2000 h at 0.2 m A cm^(-2). The ASSLSB also shows a stable cycling performance of 500 cycles at 0.5 C.This work reveals the structure–activity relationship between the mechanical property of interface layer and the battery's cycling stability.

关 键 词：All-solid-state lithium-sulfur batteries PEO-based electrolyte SEI layer High modulus Long cycling stability 

分 类 号：TM912[电气工程—电力电子与电力传动]