Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes

Jun-Hyuk Song, Seungju Yu, Byunghoon Kim, Donggun Eum, Jiung Cho, Ho-Young Jang, Sung-O Park, Jaekyun Yoo, Youngmin Ko, Kyeongsu Lee, Myeong Hwan Lee, Byungwook Kang and Kisuk Kang ()
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Jun-Hyuk Song: Seoul National University
Seungju Yu: Seoul National University
Byunghoon Kim: Seoul National University
Donggun Eum: Seoul National University
Jiung Cho: Korea Basic Science Institute
Ho-Young Jang: Seoul National University
Sung-O Park: Seoul National University
Jaekyun Yoo: Seoul National University
Youngmin Ko: Seoul National University
Kyeongsu Lee: Seoul National University
Myeong Hwan Lee: Seoul National University
Byungwook Kang: Seoul National University
Kisuk Kang: Seoul National University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Lithium-rich layered oxides, despite their potential as high-energy-density cathode materials, are impeded by electrochemical performance deterioration upon anionic redox. Although this deterioration is believed to primarily result from structural disordering, our understanding of how it is triggered and/or occurs remains incomplete. Herein, we propose a theoretical picture that clarifies the irreversible transformation and redox asymmetry of lithium-rich layered oxides by introducing a series of global and local dynamic structural evolution processes involving slab gliding and transition-metal migration. We show that slab gliding plays a key role in trigger/initiating the structural disordering and consequent degradation of the anionic redox reaction. We further reveal that the ‘concerted disordering mechanism’ of slab gliding and transition-metal migration produces spontaneously irreversible/asymmetric lithiation and de-lithiation pathways, causing irreversible structural deterioration and the asymmetry of the anionic redox reaction. Our findings suggest slab gliding as a crucial, yet underexplored, method for achieving a reversible anionic redox reaction.

Date: 2023
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DOI: 10.1038/s41467-023-39838-y

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