Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes
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...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-39838-y |
| _version_ | 1827899743822413824 |
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| author | 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 Kisuk Kang |
| author_facet | 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 Kisuk Kang |
| author_sort | Jun-Hyuk Song |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-12T23:21:55Z |
| format | Article |
| id | doaj.art-089f6630aa3347119636bbfbc8c89cef |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-12T23:21:55Z |
| publishDate | 2023-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-089f6630aa3347119636bbfbc8c89cef2023-07-16T11:21:30ZengNature PortfolioNature Communications2041-17232023-07-0114111010.1038/s41467-023-39838-ySlab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodesJun-Hyuk Song0Seungju Yu1Byunghoon Kim2Donggun Eum3Jiung Cho4Ho-Young Jang5Sung-O Park6Jaekyun Yoo7Youngmin Ko8Kyeongsu Lee9Myeong Hwan Lee10Byungwook Kang11Kisuk Kang12Department of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityWestern Seoul Center, Korea Basic Science InstituteDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityDepartment of Materials Science and Engineering, Research Institute of Advanced Materials (RIAM), Seoul National UniversityAbstract 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.https://doi.org/10.1038/s41467-023-39838-y |
| spellingShingle | 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 Kisuk Kang Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes Nature Communications |
| title | Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes |
| title_full | Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes |
| title_fullStr | Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes |
| title_full_unstemmed | Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes |
| title_short | Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes |
| title_sort | slab gliding a hidden factor that induces irreversibility and redox asymmetry of lithium rich layered oxide cathodes |
| url | https://doi.org/10.1038/s41467-023-39838-y |
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