Journal article

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


Authors listZuo, TT; Rueß, R; Pan, RJ; Walther, F; Rohnke, M; Hori, S; Kanno, R; Schröder, D; Janek, J

Publication year2021

Pages6669-

JournalNature Communications

Volume number12

Issue number1

Open access statusGold

DOI Linkhttps://doi.org/10.1038/s41467-021-26895-4

PublisherNature Research


Abstract
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.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 < 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.


Citation Styles

Harvard Citation styleZuo, T., Rueß, R., Pan, R., Walther, F., Rohnke, M., Hori, S., et al. (2021) A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries, Nature Communications, 12(1), p. 6669. https://doi.org/10.1038/s41467-021-26895-4

APA Citation styleZuo, T., Rueß, R., Pan, R., Walther, F., Rohnke, M., Hori, S., Kanno, R., Schröder, D., & Janek, J. (2021). A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries. Nature Communications. 12(1), 6669. https://doi.org/10.1038/s41467-021-26895-4


Last updated on 2025-10-06 at 11:32