Boosting Ion Conduction and Moisture Stability Through Zn2+ Substitution of Chloride Electrolytes for All-Solid-State Lithium Batteries

作     者：Lei, Peng Wu, Gang Liu, Hong Qi, Xiang Wu, Meng Li, Dabing Li, Yang Gao, Lei Nan, Ce-Wen Fan, Li-Zhen 

作者机构：Beijing Key Laboratory for Advanced Energy Materials and Technologies Institute of Advanced Materials and Technology University of Science and Technology Beijing Beijing100083 China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China 

出 版 物：《Advanced Energy Materials》 (Adv. Energy Mater.)

年 卷 期：2025年第0期

核心收录：

学科分类：0808[工学-电气工程] 070207[理学-光学] 07[理学] 0806[工学-冶金工程] 0817[工学-化学工程与技术] 08[工学] 0703[理学-化学] 0803[工学-光学工程] 0702[理学-物理学] 

基　　金：P.L. and G.W. contributed equally to this work. Financial supports from the National Natural Scientific Foundation of China (22479009 and U21A2080)  National related project  and the Fundamental Research Funds for the Central Universities (FRF\u2010TP\u201022\u201001C2) are gratefully acknowledged 

主　　题：Solid State Batteries 

摘      要：The recently emerged chloride solid electrolytes have garnered significant attention due to their superior ionic conductivity, wide electrochemical stability window, and exceptional compatibility with high-voltage oxide cathodes. Nevertheless, the currently cost-effective Zr-based chloride solid electrolytes face significant challenges, including low ionic conductivity and poor moisture stability. Herein, a versatile Zn2+-doped Zr-based chloride electrolyte is presented, designed to meet the aforementioned requirements. The optimized Li2.4Zr0.8Zn0.2Cl6 exhibits an improved ionic conductivity of 1.13 mS cm−1 at 30 °C. Simultaneously, the Li2.4Zr0.8Zn0.2Cl6 also demonstrates impressive moisture stability, maintaining its structural integrity after exposure to humid air. The mechanism underlying the enhanced moisture stability of Li2.4Zr0.8Zn0.2Cl6 is further elucidated by density functional theory calculations. Most notably, whether coupled with LiCoO2 or LiNi0.8Mn0.1Co0.1O2 cathodes, Li2.4Zr0.8Zn0.2Cl6-based all-solid-state batteries demonstrate exceptional cycling stability and rate performance. This high ionic conduction and moisture-resistant chloride electrolyte holds great promise for significantly advancing the commercialization of all-solid-state lithium batteries. © 2025 Wiley-VCH GmbH.