The nature and suppression strategies of interfacial reactions in all-solid-state batteries

Ren, Fucheng; Liang, Ziteng; Zhao, Wengao; Zuo, Wenhua; Lin, Min; Wu, Yuqi; Yang, Xuerui; Gong, Zhengliang; Yang, Yong

doi:10.1039/d3ee00870c

Title: The nature and suppression strategies of interfacial reactions in all-solid-state batteries

Journal Article · 21 April 2023 · Energy & Environmental Science

DOI: https://doi.org/10.1039/d3ee00870c · OSTI ID:1993574

Ren, Fucheng ^[1]; Liang, Ziteng ^[1];

^[2];

^[3]; Lin, Min ^[1]; Wu, Yuqi ^[1]; Yang, Xuerui ^[1];

^[1];

^[1]

Xiamen Univ. (China)
Karlsruhe Inst. of Technology (KIT) (Germany)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Solid-state Li batteries are promising energy storage devices owing to their high safety and high theoretical energy density. However, the serious interfacial reaction between solid state electrolytes and cathodes deteriorates the battery performance, impeding the realization of long-term cyclability. The buried nature of the interphase layer presents a significant challenge in achieving a comprehensive understanding of the underlying interfacial reaction mechanisms. Herein, we systematically explore the interfacial reaction evolutions and interphase compositions and electronic properties between the popular oxide cathodes and sulfide solid electrolytes (SSEs). This includes analysis of the chemical and electrochemical reactions between cathodes/coatings and SSEs, as well as the electrochemical self-decomposition of SSEs by thermodynamic phase equilibrium analysis. Herein, we disclose that the driving force of the electrochemical reaction at the chemical potential of μ_Li is much stronger than that of the chemical reaction, which dominates the interfacial reaction. Preventing the formation of an electronically conductive interphase is crucial in inhibiting the continuous interfacial degradation during long-term cycling, which can be achieved through the optimized combination of cathodes and SSEs, as well as the introduction of functional coatings between them. Based on these findings, the percentage of molar fraction (f) of electronically conductive species in the formed interphase is proposed as a key factor for indicating the interfacial stability for the first time. Furthermore, we propose a specific high-throughput screening scheme to filter the functional coating materials by comprehensively evaluating their functionality. The tiered screening identifies 48 coating materials with optimal properties. The work highlights the significant roles of rational coupling of the cathodes and SSEs, and optimizing interfacial coating materials for solid-state batteries. It opens new avenues for engineering an interphase with improved interfacial compatibility to realize long-term cyclability.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China

Grant/Contract Number:: AC02-06CH11357; 22261160570; 21935009; 22279108; 2021YFB2401800

OSTI ID:: 1993574

Journal Information:: Energy & Environmental Science, Vol. 16, Issue 6; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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