Design of a trigonal halide superionic conductor by regulating cation order-disorder

• 成果类型: Article
• 署名作者: Yu, Seungju; Noh, Joohyeon; Kim, Byunghoon; Song, Jun-Hyuk; Oh, Kyungbae; Yoo, Jaekyun; Lee, Sunyoung; Park, Sung-O; Kim, Wonju; Kang, Byungwook; Kil, Donghyun; Kang, Kisuk
• 署名单位: Seoul National University (SNU); Samsung; Samsung Display; Seoul National University (SNU); Institute for Basic Science - Korea (IBS); Seoul National University (SNU); Seoul National University (SNU)
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8196
• DOI: 10.1126/science.adg6591
• 发表日期: 2023-11-03
• 页码: 573-579
• 关键词: solid-state electrolytes; lithium; DYNAMICS; interface; oxides; plane

摘要

Lithium-metal-halides have emerged as a class of solid electrolytes that can deliver superionic conductivity comparable to that of state-of-the-art sulfide electrolytes, as well as electrochemical stability that is suitable for high-voltage (>4 volt) operations. We show that the superionic conduction in a trigonal halide, such as Li3MCl6 [where metal (M) is Y or Er], is governed by the in-plane lithium percolation paths and stacking interlayer distance. These two factors are inversely correlated with each other by the partial occupancy of M, serving as both a diffusion inhibitor and pillar for maintaining interlayer distance. These findings suggest that a critical range or ordering of M exists in trigonal halides, and we showcase the achievement of high ionic conductivity by adjusting the simple M ratio (per Cl or Li). We provide general design criteria for superionic trigonal halide electrolytes.