A theoretical framework for oxygen redox chemistry for sustainable batteries

Byunghoon Kim, Jun-Hyuk Song, Donggun Eum, Seungju Yu, Kyungbae Oh, Myeong Hwan Lee, Ho-Young Jang and Kisuk Kang ()
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Byunghoon Kim: Research Institute of Advanced Materials (RIAM), Seoul National University
Jun-Hyuk Song: Research Institute of Advanced Materials (RIAM), Seoul National University
Donggun Eum: Research Institute of Advanced Materials (RIAM), Seoul National University
Seungju Yu: Research Institute of Advanced Materials (RIAM), Seoul National University
Kyungbae Oh: Research Institute of Advanced Materials (RIAM), Seoul National University
Myeong Hwan Lee: Research Institute of Advanced Materials (RIAM), Seoul National University
Ho-Young Jang: Research Institute of Advanced Materials (RIAM), Seoul National University
Kisuk Kang: Research Institute of Advanced Materials (RIAM), Seoul National University

Nature Sustainability, 2022, vol. 5, issue 8, 708-716

Abstract: Abstract Lithium-rich layered oxides have emerged as a new model for designing the next generation of cathode materials for batteries to assist the transition to a greener energy system. The unique oxygen redox mechanism of such cathodes enables extra energy storage capacity beyond the contribution from merely transition metal ions; however, their practical application is hindered by the destabilizing structural changes during operation. Here we present a theoretical framework for the triptych of structural disorder, bond covalency and oxygen redox chemistry that applies to a wide range of layered oxides. It is revealed that structural disorder stabilizes the oxygen redox by promoting the formation of oxygen covalent bonds in favour of electrochemical reversibility. Oxygen dimers are found to move freely within the lattice structure and serve as a key catalyst of the poor structural resilience. Such fundamental understanding provides fresh insights that could inform strategies to mitigate the limitations of anionic redox cathodes, moving us a step closer to tapping into their enormous potential.

Date: 2022
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DOI: 10.1038/s41893-022-00890-z

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