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A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries
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A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries
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Journal Article
A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries
2021
Overview
All-solid-state batteries are intensively investigated, although their performance is not yet satisfactory for large-scale applications. In this context, the combination of Li
10
GeP
2
S
12
solid electrolyte and LiNi
1-x-y
Co
x
Mn
y
O
2
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 <
E
< 4.2 V
vs
. Li
+
/Li) and high (
E
≥ 4.2 V
vs
. Li
+
/Li) potentials. A high state of charge (>80%) triggers the structural instability and oxygen release at the positive electrode and leads to more severe degradation.
Fundamental investigations at the electrode/electrolyte interface are essential for developing high-energy batteries. Here, the authors investigate the degradation mechanisms at the LGPS/NCM622 interface providing a quantitative model to interpret the interfacial resistance growth.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
