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Hidden structural and chemical order controls lithium transport in cation-disordered oxides for rechargeable batteries

Author

Listed:
  • Huiwen Ji

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Alexander Urban

    (University of California Berkeley
    Lawrence Berkeley National Laboratory
    University of St Andrews)

  • Daniil A. Kitchaev

    (Massachusetts Institute of Technology)

  • Deok-Hwang Kwon

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Nongnuch Artrith

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Colin Ophus

    (Lawrence Berkeley National Laboratory)

  • Wenxuan Huang

    (Massachusetts Institute of Technology)

  • Zijian Cai

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Tan Shi

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Jae Chul Kim

    (Lawrence Berkeley National Laboratory
    Stevens Institute of Technology)

  • Haegyeom Kim

    (Lawrence Berkeley National Laboratory)

  • Gerbrand Ceder

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

Abstract

Structure plays a vital role in determining materials properties. In lithium ion cathode materials, the crystal structure defines the dimensionality and connectivity of interstitial sites, thus determining lithium ion diffusion kinetics. In most conventional cathode materials that are well-ordered, the average structure as seen in diffraction dictates the lithium ion diffusion pathways. Here, we show that this is not the case in a class of recently discovered high-capacity lithium-excess rocksalts. An average structure picture is no longer satisfactory to understand the performance of such disordered materials. Cation short-range order, hidden in diffraction, is not only ubiquitous in these long-range disordered materials, but fully controls the local and macroscopic environments for lithium ion transport. Our discovery identifies a crucial property that has previously been overlooked and provides guidelines for designing and engineering cation-disordered cathode materials.

Suggested Citation

  • Huiwen Ji & Alexander Urban & Daniil A. Kitchaev & Deok-Hwang Kwon & Nongnuch Artrith & Colin Ophus & Wenxuan Huang & Zijian Cai & Tan Shi & Jae Chul Kim & Haegyeom Kim & Gerbrand Ceder, 2019. "Hidden structural and chemical order controls lithium transport in cation-disordered oxides for rechargeable batteries," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08490-w
    DOI: 10.1038/s41467-019-08490-w
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    Cited by:

    1. Kit McColl & Robert A. House & Gregory J. Rees & Alexander G. Squires & Samuel W. Coles & Peter G. Bruce & Benjamin J. Morgan & M. Saiful Islam, 2022. "Transition metal migration and O2 formation underpin voltage hysteresis in oxygen-redox disordered rocksalt cathodes," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    2. Linze Li & Bin Ouyang & Zhengyan Lun & Haoyan Huo & Dongchang Chen & Yuan Yue & Colin Ophus & Wei Tong & Guoying Chen & Gerbrand Ceder & Chongmin Wang, 2023. "Atomic-scale probing of short-range order and its impact on electrochemical properties in cation-disordered oxide cathodes," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Hui Liu & Xiaoming Shi & Yonghao Yao & Huajie Luo & Qiang Li & Houbing Huang & He Qi & Yuanpeng Zhang & Yang Ren & Shelly D. Kelly & Krystian Roleder & Joerg C. Neuefeind & Long-Qing Chen & Xianran Xi, 2023. "Emergence of high piezoelectricity from competing local polar order-disorder in relaxor ferroelectrics," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Zijian Cai & Bin Ouyang & Han-Ming Hau & Tina Chen & Raynald Giovine & Krishna Prasad Koirala & Linze Li & Huiwen Ji & Yang Ha & Yingzhi Sun & Jianping Huang & Yu Chen & Vincent Wu & Wanli Yang & Chon, 2024. "In situ formed partially disordered phases as earth-abundant Mn-rich cathode materials," Nature Energy, Nature, vol. 9(1), pages 27-36, January.
    5. Yuta Yasui & Masataka Tansho & Kotaro Fujii & Yuichi Sakuda & Atsushi Goto & Shinobu Ohki & Yuuki Mogami & Takahiro Iijima & Shintaro Kobayashi & Shogo Kawaguchi & Keiichi Osaka & Kazutaka Ikeda & Tos, 2023. "Hidden chemical order in disordered Ba7Nb4MoO20 revealed by resonant X-ray diffraction and solid-state NMR," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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