journal article·2024-09Open access

Regulating Ion Diffusion and Stability in Amorphous Thiosilicate‐Based Solid Electrolytes Through Edge‐Sharing Local Structures

Xiaoge Hao, James A. Quirk, Feipeng Zhao, Sandamini H Alahakoon, Jiabin Ma, Jiamin Fu, Jung Tae Kim, Weihan Li, Minsi Li, Shumin Zhang, Hui Duan, Yining Huang, James A. Dawson, Xueliang Sun

Advanced Energy Materials· Volume 14· Issue 35

Abstract

Abstract Amorphous solid‐state electrolytes (SSEs) play a pivotal role as fundamental components within all‐solid‐state lithium batteries, yet their understanding lags behind that of crystalline materials. In this work, a novel amorphous SSE 5Li2S‐3SiS2 (mol %) with a high ionic conductivity of 1.2 mS cm−1 is first reported. The silicon and sulfur atoms in the edge‐sharing Si2S64− are less attracted to lithium compared to the SiS44− anion, which is expected to facilitate the lithium ions conduction in SSEs. More importantly, the relationship between the material properties and local structure in the amorphous thiosilicate SSEs is revealed, particularly highlighting the desirable edge‐sharing local structure. The Si2S64− presents better stability with Li metal. This work offers an important guideline in the development of anion frameworks in amorphous sulfide SSEs for high‐performance all‐solid‐state lithium metal batteries.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Thermal Expansion and Ionic Conductivity · Advancements in Battery Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Mechanical and Materials Engineering University of Western Ontario London Ontario N6A 5B9 Canada

Chemistry – School of Natural and Environmental Sciences Newcastle University Newcastle upon Tyne NE1 7RU UK

Department of Chemistry University of Western Ontario London Ontario N6A 5B7 Canada

Shenzhen Geim Graphene Center Tsinghua‐Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 P. R. China

Eastern Institute for Advanced Study Eastern Institute of Technology Ningbo Zhejiang 315201 P. R. China

Funding

Canada Foundation for Innovation · University of Saskatchewan · Engineering and Physical Sciences Research Council

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