Size-Dependent Chemomechanical Failure of Sulfide Solid Electrolyte Particles during Electrochemical Reaction with Lithium

Jun Zhao; Chao Zhao; Jianping Zhu; Xiangsi Liu; Jingming Yao; Bo Wang; Qiushi Dai; Zaifa Wang; Jingzhao Chen; Peng Jia; Yanshuai Li; Stephen J Harris; Yong Yang; Yongfu Tang; Liqiang Zhang; Feng Ding; Jianyu Huang

doi:10.1021/acs.nanolett.1c04076

Size-Dependent Chemomechanical Failure of Sulfide Solid Electrolyte Particles during Electrochemical Reaction with Lithium

Nano Lett. 2022 Jan 12;22(1):411-418. doi: 10.1021/acs.nanolett.1c04076. Epub 2021 Dec 23.

Authors

Jun Zhao¹, Chao Zhao², Jianping Zhu³, Xiangsi Liu³, Jingming Yao¹, Bo Wang¹, Qiushi Dai¹, Zaifa Wang¹, Jingzhao Chen¹, Peng Jia¹, Yanshuai Li¹, Stephen J Harris⁴, Yong Yang³, Yongfu Tang^{1

5}, Liqiang Zhang¹, Feng Ding², Jianyu Huang^{1

6}

Affiliations

¹ Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, P.R. China.
² Institute for Basic Science (IBS), School of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea.
³ Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory for Physical Chemistry of Solid Surface, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P.R. China.
⁴ Energy Storage Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
⁵ Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, P.R. China.
⁶ School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan 411105, P.R. China.

PMID: 34941277
DOI: 10.1021/acs.nanolett.1c04076

Abstract

The very high ionic conductivity of Li₁₀GeP₂S₁₂ (LGPS) solid electrolyte (SE) makes it a promising candidate SE for solid-state batteries in electrical vehicles. However, chemomechanical failure, whose mechanism remains unclear, has plagued its widespread applications. Here, we report in situ imaging lithiation-induced failure of LGPS SE. We revealed a strong size effect in the chemomechanical failure of LGPS particles: namely, when the particle size is greater than 3 μm, fracture/pulverization occurred; when the particle size is between 1 and 3 μm, microcracks emerged; when the particle size is less than 1 μm, no chemomechanical failure was observed. This strong size effect is interpreted by the interplay between elastic energy storage and dissipation. Our finding has important implications for the design of high-performance LGPS SE, for example, by reducing the particle size to less than 1 μm the chemomechanical failure of LGPS SE can be mitigated.

Keywords: Chemomechanical failure; Size effect; Solid-state batteries; Sulfide solid electrolyte.