IDEAS home Printed from https://ideas.repec.org/a/nat/nature/v606y2022i7913d10.1038_s41586-022-04689-y.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41586-022-04689-y
    File Function: Abstract
    Download Restriction: Access to the full text of the articles in this series is restricted.

    File URL: https://libkey.io/10.1038/s41586-022-04689-y?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    As the access to this document is restricted, you may want to search for a different version of it.

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. 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.
    2. 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.
    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. Tonghuan Yang & Kun Zhang & Yuxuan Zuo & Jin Song & Yali Yang & Chuan Gao & Tao Chen & Hangchao Wang & Wukun Xiao & Zewen Jiang & Dingguo Xia, 2024. "Ultrahigh-nickel layered cathode with cycling stability for sustainable lithium-ion batteries," Nature Sustainability, Nature, vol. 7(9), pages 1204-1214, September.
    5. 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.
    6. 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.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:nature:v:606:y:2022:i:7913:d:10.1038_s41586-022-04689-y. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.