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A theoretical framework for oxygen redox chemistry for sustainable batteries

Author

Listed:
  • Byunghoon Kim

    (Research Institute of Advanced Materials (RIAM), Seoul National University
    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
    Seoul National University
    Seoul National University
    Seoul National University)

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.

Suggested Citation

  • Byunghoon Kim & Jun-Hyuk Song & Donggun Eum & Seungju Yu & Kyungbae Oh & Myeong Hwan Lee & Ho-Young Jang & Kisuk Kang, 2022. "A theoretical framework for oxygen redox chemistry for sustainable batteries," Nature Sustainability, Nature, vol. 5(8), pages 708-716, August.
    • Handle: RePEc:nat:natsus:v:5:y:2022:i:8:d:10.1038_s41893-022-00890-z
    DOI: 10.1038/s41893-022-00890-z
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    Cited by:

    1. Zhongsheng Dai & Zhujie Li & Renjie Chen & Feng Wu & Li Li, 2023. "Defective oxygen inert phase stabilized high-voltage nickel-rich cathode for high-energy lithium-ion batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Hanrui Zhang & Ying Han & Jianwei Lai & Joseph Wolf & Zhen Lei & Yang Yang & Feifei Shi, 2024. "Direct extraction of lithium from ores by electrochemical leaching," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. 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, 2023. "Slab gliding, a hidden factor that induces irreversibility and redox asymmetry of lithium-rich layered oxide cathodes," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Ho-Young Jang & Donggun Eum & Jiung Cho & Jun Lim & Yeji Lee & Jun-Hyuk Song & Hyeokjun Park & Byunghoon Kim & Do-Hoon Kim & Sung-Pyo Cho & Sugeun Jo & Jae Hoon Heo & Sunyoung Lee & Jongwoo Lim & Kisu, 2024. "Structurally robust lithium-rich layered oxides for high-energy and long-lasting cathodes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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