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In situ formed partially disordered phases as earth-abundant Mn-rich cathode materials

Author

Listed:
  • Zijian Cai

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Bin Ouyang

    (Florida State University)

  • Han-Ming Hau

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Tina Chen

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Raynald Giovine

    (University of California Santa Barbara
    University of California Santa Barbara)

  • Krishna Prasad Koirala

    (Pacific Northwest National Laboratory)

  • Linze Li

    (Pacific Northwest National Laboratory)

  • Huiwen Ji

    (University of Utah)

  • Yang Ha

    (Lawrence Berkeley National Laboratory)

  • Yingzhi Sun

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Jianping Huang

    (Lawrence Berkeley National Laboratory)

  • Yu Chen

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Vincent Wu

    (University of California Santa Barbara
    University of California Santa Barbara)

  • Wanli Yang

    (Lawrence Berkeley National Laboratory)

  • Chongmin Wang

    (Pacific Northwest National Laboratory)

  • Raphaële J. Clément

    (University of California Santa Barbara
    University of California Santa Barbara)

  • Zhengyan Lun

    (University of California Berkeley
    Lawrence Berkeley National Laboratory
    University of Chinese Academy of Sciences)

  • Gerbrand Ceder

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

Abstract

Earth-abundant cathode materials are urgently needed to enable scaling of the Li-ion industry to multiply terawatt hours of annual production, necessitating reconsideration of how good cathode materials can be obtained. Irreversible transition metal migration and phase transformations in Li-ion cathodes are typically believed to be detrimental because they may trigger voltage hysteresis, poor kinetics and capacity degradation. Here we challenge this conventional consensus by reporting an unusual phase transformation from disordered Li- and Mn-rich rock salts to a new phase (named δ), which displays partial spinel-like ordering with short coherence length and exhibits high energy density and rate capability. Unlike other Mn-based cathodes, the δ phase exhibits almost no voltage fade upon cycling. We identify the driving force and kinetics of this in situ cathode formation and establish design guidelines for Li- and Mn-rich compositions that combine high energy density, high rate capability and good cyclability, thereby enabling Mn-based energy storage.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natene:v:9:y:2024:i:1:d:10.1038_s41560-023-01375-9
    DOI: 10.1038/s41560-023-01375-9
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    References listed on IDEAS

    as
    1. Gaurav Assat & Jean-Marie Tarascon, 2018. "Fundamental understanding and practical challenges of anionic redox activity in Li-ion batteries," Nature Energy, Nature, vol. 3(5), pages 373-386, May.
    2. Huiwen Ji & Jinpeng Wu & Zijian Cai & Jue Liu & Deok-Hwang Kwon & Hyunchul Kim & Alexander Urban & Joseph K. Papp & Emily Foley & Yaosen Tian & Mahalingam Balasubramanian & Haegyeom Kim & Raphaële J. , 2020. "Ultrahigh power and energy density in partially ordered lithium-ion cathode materials," Nature Energy, Nature, vol. 5(3), pages 213-221, March.
    3. Weibo Hua & Suning Wang & Michael Knapp & Steven J. Leake & Anatoliy Senyshyn & Carsten Richter & Murat Yavuz & Joachim R. Binder & Clare P. Grey & Helmut Ehrenberg & Sylvio Indris & Björn Schwarz, 2019. "Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    4. 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.
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