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Electrochemomechanical failure in layered oxide cathodes caused by rotational stacking faults

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Title
Electrochemomechanical failure in layered oxide cathodes caused by rotational stacking faults
Author(s)
Donggun Eum; Park, Sung-O; Jang, Ho-Young; Jeon, Youngjun; Song, Jun-Hyuk; Han, Sangwook; Kim, Kyoungoh; Kisuk Kang
Publication Date
2024-08
Journal
Nature Materials, v.23, pp.1093 - 1099
Publisher
Nature Publishing Group
Abstract
Electrochemomechanical degradation is one of the most common causes of capacity deterioration in high-energy-density cathodes, particularly intercalation-based layered oxides. Here we reveal the presence of rotational stacking faults (RSFs) in layered lithium transition-metal oxides, arising from specific stacking sequences at different angles, and demonstrate their critical role in determining structural/electrochemical stability. Our combined experiments and calculations show that RSFs facilitate oxygen dimerization and transition-metal migration in layered oxides, fostering microcrack nucleation/propagation concurrently with cumulative electrochemomechanical degradation on cycling. We further show that thermal defect annihilation as a potential solution can suppress RSFs, reducing microcracks and enhancing cyclability in lithium-rich layered cathodes. The common but previously overlooked occurrence of RSFs suggests a new synthesis guideline of high-energy-density layered oxide cathodes. © The Author(s), under exclusive licence to Springer Nature Limited 2024.
URI
https://pr.ibs.re.kr/handle/8788114/15461
DOI
10.1038/s41563-024-01899-9
ISSN
1476-1122
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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