A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries

Tong-Tong Zuo (), Raffael Rueß, Ruijun Pan, Felix Walther, Marcus Rohnke, Satoshi Hori, Ryoji Kanno, Daniel Schröder () and Jürgen Janek ()
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Tong-Tong Zuo: Justus Liebig University Giessen
Raffael Rueß: Justus Liebig University Giessen
Ruijun Pan: Justus Liebig University Giessen
Felix Walther: Justus Liebig University Giessen
Marcus Rohnke: Justus Liebig University Giessen
Satoshi Hori: Tokyo Institute of Technology
Ryoji Kanno: Tokyo Institute of Technology
Daniel Schröder: Technische Universität Braunschweig
Jürgen Janek: Justus Liebig University Giessen

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract All-solid-state batteries are intensively investigated, although their performance is not yet satisfactory for large-scale applications. In this context, the combination of Li10GeP2S12 solid electrolyte and LiNi1-x-yCoxMnyO2 positive electrode active materials is considered promising despite the yet unsatisfactory battery performance induced by the thermodynamically unstable electrode|electrolyte interface. Here, we report electrochemical and spectrometric studies to monitor the interface evolution during cycling and understand the reactivity and degradation kinetics. We found that the Wagner-type model for diffusion-controlled reactions describes the degradation kinetics very well, suggesting that electronic transport limits the growth of the degradation layer formed at the electrode|electrolyte interface. Furthermore, we demonstrate that the rate of interfacial degradation increases with the state of charge and the presence of two oxidation mechanisms at medium (3.7 V vs. Li+/Li 80%) triggers the structural instability and oxygen release at the positive electrode and leads to more severe degradation.

Date: 2021
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DOI: 10.1038/s41467-021-26895-4

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