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Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes
Cited 3 time in
Web of Science
Cited 3 time in Scopus
- Authors
- Issue Date
- 2023-07
- Publisher
- Nature Publishing Group
- Citation
- Nature Communications, Vol.14 No.1, p. 4149
- 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. Lithium-rich layered oxides, promising high-energy-density cathode materials, face electrochemical degradation due to structural disordering. Here, the authors report that slab gliding is a key trigger of this disordering and a pivotal unexplored avenue for a reversible anionic redox reaction.
- ISSN
- 2041-1723
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