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Origin of structural degradation in Li-rich layered oxide cathode

Author

Listed:
  • Tongchao Liu

    (Argonne National Laboratory)

  • Jiajie Liu

    (Peking University, Shenzhen Graduate School)

  • Luxi Li

    (Argonne National Laboratory)

  • Lei Yu

    (Argonne National Laboratory)

  • Jiecheng Diao

    (University College London)

  • Tao Zhou

    (Argonne National Laboratory)

  • Shunning Li

    (Peking University, Shenzhen Graduate School)

  • Alvin Dai

    (Argonne National Laboratory)

  • Wenguang Zhao

    (Peking University, Shenzhen Graduate School)

  • Shenyang Xu

    (Peking University, Shenzhen Graduate School)

  • Yang Ren

    (Argonne National Laboratory
    City University of Hong Kong)

  • Liguang Wang

    (Argonne National Laboratory)

  • Tianpin Wu

    (Argonne National Laboratory)

  • Rui Qi

    (Peking University, Shenzhen Graduate School)

  • Yinguo Xiao

    (Peking University, Shenzhen Graduate School)

  • Jiaxin Zheng

    (Peking University, Shenzhen Graduate School)

  • Wonsuk Cha

    (Argonne National Laboratory)

  • Ross Harder

    (Argonne National Laboratory)

  • Ian Robinson

    (University College London
    Brookhaven National Laboratory)

  • Jianguo Wen

    (Argonne National Laboratory)

  • Jun Lu

    (Argonne National Laboratory)

  • Feng Pan

    (Peking University, Shenzhen Graduate School)

  • Khalil Amine

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

Abstract

Li- and Mn-rich (LMR) cathode materials that utilize both cation and anion redox can yield substantial increases in battery energy density1–3. However, although voltage decay issues cause continuous energy loss and impede commercialization, the prerequisite driving force for this phenomenon remains a mystery3–6 Here, with in situ nanoscale sensitive coherent X-ray diffraction imaging techniques, we reveal that nanostrain and lattice displacement accumulate continuously during operation of the cell. Evidence shows that this effect is the driving force for both structure degradation and oxygen loss, which trigger the well-known rapid voltage decay in LMR cathodes. By carrying out micro- to macro-length characterizations that span atomic structure, the primary particle, multiparticle and electrode levels, we demonstrate that the heterogeneous nature of LMR cathodes inevitably causes pernicious phase displacement/strain, which cannot be eliminated by conventional doping or coating methods. We therefore propose mesostructural design as a strategy to mitigate lattice displacement and inhomogeneous electrochemical/structural evolutions, thereby achieving stable voltage and capacity profiles. These findings highlight the significance of lattice strain/displacement in causing voltage decay and will inspire a wave of efforts to unlock the potential of the broad-scale commercialization of LMR cathode materials.

Suggested Citation

  • Tongchao Liu & Jiajie Liu & Luxi Li & Lei Yu & Jiecheng Diao & Tao Zhou & Shunning Li & Alvin Dai & Wenguang Zhao & Shenyang Xu & Yang Ren & Liguang Wang & Tianpin Wu & Rui Qi & Yinguo Xiao & Jiaxin Z, 2022. "Origin of structural degradation in Li-rich layered oxide cathode," Nature, Nature, vol. 606(7913), pages 305-312, June.
  • Handle: RePEc:nat:nature:v:606:y:2022:i:7913:d:10.1038_s41586-022-04689-y
    DOI: 10.1038/s41586-022-04689-y
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    Citations

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    Cited by:

    1. Chuanlai Liu & Franz Roters & Dierk Raabe, 2024. "Role of grain-level chemo-mechanics in composite cathode degradation of solid-state lithium batteries," Nature Communications, Nature, vol. 15(1), pages 1-18, December.
    2. Zhichen Xue & Nikhil Sharma & Feixiang Wu & Piero Pianetta & Feng Lin & Luxi Li & Kejie Zhao & Yijin Liu, 2023. "Asynchronous domain dynamics and equilibration in layered oxide battery cathode," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    3. Tianwei Cui & Jialiang Xu & Xin Wang & Longxiang Liu & Yuxuan Xiang & Hong Zhu & Xiang Li & Yongzhu Fu, 2024. "Highly reversible transition metal migration in superstructure-free Li-rich oxide boosting voltage stability and redox symmetry," Nature Communications, Nature, vol. 15(1), pages 1-12, 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.
    5. Jonathan J. P. Peters & Tiarnan Mullarkey & Emma Hedley & Karin H. Müller & Alexandra Porter & Ali Mostaed & Lewys Jones, 2023. "Electron counting detectors in scanning transmission electron microscopy via hardware signal processing," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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