Stability Criterion for Electrodeposition in Solid-State Batteries with Metallic Anodes

作     者：Liu, Yuanpeng Zhang, Jiawei Zhang, Bowen Gao, Haowen Chen, Dongjiang Wang, Mingsheng Wang, Changguo 

作者机构：Center for Composite Materials Harbin Institute of Technology Harbin150001 China National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of Technology Harbin150080 China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen361005 China State Key Laboratory of Electronic Thin Film and Integrated Devices University of Electronic Science and Technology of China Chengdu610054 China 

出 版 物：《SSRN》 

年 卷 期：2023年

核心收录：

主　　题：Solid electrolytes 

摘      要：The application of alkali metals as anode materials for solid-state batteries essentially hinges on the fundamental study of the electrodeposition stability. Due to the absence of a complete description of electrodeposition process, it is yet unclear which factors are the most crucial for stable electrodeposition, let alone the stability criterion. Here we establish an analytical criterion for stable electrodeposition by combining electrochemistry and mechanics. In-situ experiments combined with molecular simulations are performed to validate the robustness of the theoretical predictions. Our analysis shows that the stable electrodeposition is intimately linked to the interfacial defect size, fracture toughness and molar volume of solid electrolytes. We find an exponential scaling law between the critical current density and the interfacial defect size, and the inherent softening in strength of grain boundaries lowers the critical current density in polycrystalline solid electrolytes. These modeling and analyses provide roadmaps in designing solid electrolytes with metallic anodes for achieving stable electrodeposition. © 2023, The Authors. All rights reserved.