Local charge homogenization strategy enables ultra-high voltage tolerance of polyether electrolytes for 4.7 V lithium metal batteries  

作　　者：Yuanlong Wu Piao Luo Kexin Su Mao Yu Xin Song Lianzhan Huang Shaocong Zhang Huiyu Song Li Du Weishu Liu Zhiming Cui 

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 510641,China [2]Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen 518055,China [3]Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials,School of Materials Science and Engineering,South China University of Technology,Guangzhou 510641,China [4]School of Software Engineering,South China University of Technology,Guangzhou 510006,China

出　　处：《National Science Review》2025年第2期213-223,共11页国家科学评论(英文版)

基　　金：supported by the National Natural Science Foundation of China(NSFC,22372062);the Key Technologies R&D Program of Guangdong Province(2023B0909060003);the support of the NSFC Program for Distinguished Young Scholars(T2425012);the Shen-Zhen Innovation Program for Distinguished Young Scholars(RCJC20210706091949018).

摘　　要：In-situ fabricated polyether electrolytes have been regarded as one of the most promising solid electrolyte systems.Nevertheless,they cannot match high-voltage cathodes over 4.3 V due to their poor oxidative stability.Herein,we propose an effective local charge homogenization strategy based on the triglycidyl isocyanurate(TGIC)crosslinker,achieving ultra-high-voltage electrochemical stability of polyether electrolytes(viz.PTIDOL)at cutoffvoltages up to 4.7 V.The introduction of TGIC optimizes the Li^(+)solvation environment,thereby homogenizing the charge distribution at ether oxygen(EO)sites,resulting in significantly enhanced oxidative stability of the polyether main chain.Consequently,the Li|PTIDOL|LiNi_(0.6) Co_(0.2) Mn_(0.2) O_(2)(NCM622)cell achieves long-term operation at an ultra-high cutoffvoltage with a capacity retention of 81.8%after 400 cycles,one of the best results reported for polyether electrolytes to date.This work provides significant insights for the development of polyether electrolytes with high-voltage tolerance and the advancement of high-energy-density batteries.

关 键 词：lithium metal batteries solid polymer electrolytes in-situ polymerization high voltage local charge homogenization 

分 类 号：O63[理学—高分子化学]