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

Lookup NU author(s): Dr James Quirk, Dr James DawsonORCiD

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This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License (CC BY-NC-ND).


Abstract

© 2024 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH. 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.


Publication metadata

Author(s): Hao X, Quirk JA, Zhao F, Alahakoon SH, Ma J, Fu J, Kim JT, Li W, Li M, Zhang S, Duan H, Huang Y, Dawson JA, Sun X

Publication type: Article

Publication status: Published

Journal: Advanced Energy Materials

Year: 2024

Pages: ePub ahead of Print

Online publication date: 16/06/2024

Acceptance date: 30/05/2024

Date deposited: 25/06/2024

ISSN (print): 1614-6832

ISSN (electronic): 1614-6840

Publisher: John Wiley and Sons Inc.

URL: https://doi.org/10.1002/aenm.202304556

DOI: 10.1002/aenm.202304556

Data Access Statement: The data that support the ?ndings of this study are available from the corresponding author upon reasonable request.


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Funding

Funder referenceFunder name
Canada Foundation for Innovation (CFI)
Canada Light Source (CLS) at the University of Saskatchewan
Canada Research Chair Program
EP/V013130/1
EPSRC
Nature Sciences and Engineering Research Council of Canada (NSERC)
Ontario Research Fund
University of Western Ontario

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