First principles study on electrochemical and chemical stability of solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries

Zhu, Yizhou; He, Xingfeng; Mo, Yifei

doi:10.1039/c5ta08574h

First principles study on electrochemical and chemical stability of solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries

Journal Article · Fri Dec 11 00:00:00 EST 2015 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/c5ta08574h· OSTI ID:1433677

Zhu, Yizhou ^[1]; He, Xingfeng ^[2]; Mo, Yifei ^[3]

Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering; University of Maryland, College Park
Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering
Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering. Energy Research Center

All-solid-state Li-ion batteries based on ceramic solid electrolyte materials are a promising next-generation energy storage technology with high energy density and enhanced cycle life. The poor interfacial conductance is one of the key limitations in enabling all-solid-state Li-ion batteries. However, the origin of this poor conductance has not been understood, and there is limited knowledge about the solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries. In this paper, we performed first principles calculations to evaluate the thermodynamics of the interfaces between solid electrolyte and electrode materials and to identify the chemical and electrochemical stabilities of these interfaces. Our computation results reveal that many solid electrolyte–electrode interfaces have limited chemical and electrochemical stability, and that the formation of interphase layers is thermodynamically favorable at these interfaces. These formed interphase layers with different properties significantly affect the electrochemical performance of all-solid-state Li-ion batteries. The mechanisms of applying interfacial coating layers to stabilize the interface and to reduce interfacial resistance are illustrated by our computation. This study demonstrates a computational scheme to evaluate the chemical and electrochemical stability of heterogeneous solid interfaces. Finally, the enhanced understanding of the interfacial phenomena provides the strategies of interface engineering to improve performances of all-solid-state Li-ion batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Maryland, College Park, MD (United States)

Sponsoring Organization:: National Science Foundation (NSF) (United States); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: EE0006860

OSTI ID:: 1433677

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 9 Vol. 4; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Electrochemical Stability of Li₁₀GeP₂S₁₂ and Li₇La₃Zr₂O₁₂ Solid Electrolytes

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First principles study on electrochemical and chemical stability of solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries

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