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Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Author

Listed:
  • Xiang Liu

    (Argonne National Laboratory)

  • Gui-Liang Xu

    (Argonne National Laboratory)

  • Venkata Surya Chaitanya Kolluru

    (Argonne National Laboratory
    University of Florida)

  • Chen Zhao

    (Argonne National Laboratory)

  • Qingtian Li

    (Lawrence Berkeley National Laboratory)

  • Xinwei Zhou

    (Argonne National Laboratory)

  • Yuzi Liu

    (Argonne National Laboratory)

  • Liang Yin

    (Argonne National Laboratory)

  • Zengqing Zhuo

    (Lawrence Berkeley National Laboratory)

  • Amine Daali

    (Argonne National Laboratory)

  • Jing-Jing Fan

    (Xiamen University)

  • Wenjun Liu

    (Argonne National Laboratory)

  • Yang Ren

    (Argonne National Laboratory)

  • Wenqian Xu

    (Argonne National Laboratory)

  • Junjing Deng

    (Argonne National Laboratory)

  • Inhui Hwang

    (Argonne National Laboratory)

  • Dongsheng Ren

    (Tsinghua University)

  • Xuning Feng

    (Tsinghua University)

  • Chengjun Sun

    (Argonne National Laboratory)

  • Ling Huang

    (Xiamen University)

  • Tao Zhou

    (Argonne National Laboratory)

  • Ming Du

    (Argonne National Laboratory)

  • Zonghai Chen

    (Argonne National Laboratory)

  • Shi-Gang Sun

    (Xiamen University)

  • Maria K. Y. Chan

    (Argonne National Laboratory)

  • Wanli Yang

    (Lawrence Berkeley National Laboratory)

  • Minggao Ouyang

    (Tsinghua University)

  • Khalil Amine

    (Argonne National Laboratory
    Stanford University
    Mohammed VI Polytechnic University (UM6P))

Abstract

Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.

Suggested Citation

  • Xiang Liu & Gui-Liang Xu & Venkata Surya Chaitanya Kolluru & Chen Zhao & Qingtian Li & Xinwei Zhou & Yuzi Liu & Liang Yin & Zengqing Zhuo & Amine Daali & Jing-Jing Fan & Wenjun Liu & Yang Ren & Wenqia, 2022. "Origin and regulation of oxygen redox instability in high-voltage battery cathodes," Nature Energy, Nature, vol. 7(9), pages 808-817, September.
    • Handle: RePEc:nat:natene:v:7:y:2022:i:9:d:10.1038_s41560-022-01036-3
    DOI: 10.1038/s41560-022-01036-3
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    Citations

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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. 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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