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Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials

Author

Listed:
  • Jinhyuk Lee

    (University of California
    Massachusetts Institute of Technology)

  • Daniil A. Kitchaev

    (Massachusetts Institute of Technology)

  • Deok-Hwang Kwon

    (University of California)

  • Chang-Wook Lee

    (Advanced Photon Source, Argonne National Laboratory)

  • Joseph K. Papp

    (University of California)

  • Yi-Sheng Liu

    (Lawrence Berkeley National Laboratory)

  • Zhengyan Lun

    (University of California)

  • Raphaële J. Clément

    (University of California)

  • Tan Shi

    (University of California)

  • Bryan D. McCloskey

    (University of California
    Lawrence Berkeley National Laboratory)

  • Jinghua Guo

    (Lawrence Berkeley National Laboratory
    University of California)

  • Mahalingam Balasubramanian

    (Advanced Photon Source, Argonne National Laboratory)

  • Gerbrand Ceder

    (University of California
    Lawrence Berkeley National Laboratory)

Abstract

There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.

Suggested Citation

  • Jinhyuk Lee & Daniil A. Kitchaev & Deok-Hwang Kwon & Chang-Wook Lee & Joseph K. Papp & Yi-Sheng Liu & Zhengyan Lun & Raphaële J. Clément & Tan Shi & Bryan D. McCloskey & Jinghua Guo & Mahalingam Balas, 2018. "Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials," Nature, Nature, vol. 556(7700), pages 185-190, April.
    • Handle: RePEc:nat:nature:v:556:y:2018:i:7700:d:10.1038_s41586-018-0015-4
    DOI: 10.1038/s41586-018-0015-4
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    Citations

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    Cited by:

    1. Huajun Tian & Guangxia Feng & Qi Wang & Zhao Li & Wei Zhang & Marcos Lucero & Zhenxing Feng & Zi-Le Wang & Yuning Zhang & Cheng Zhen & Meng Gu & Xiaonan Shan & Yang Yang, 2022. "Three-dimensional Zn-based alloys for dendrite-free aqueous Zn battery in dual-cation electrolytes," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. 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.
    3. 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.
    4. Yi Pei & Qing Chen & Meiyu Wang & Pengjun Zhang & Qingyong Ren & Jingkai Qin & Penghao Xiao & Li Song & Yu Chen & Wen Yin & Xin Tong & Liang Zhen & Peng Wang & Cheng-Yan Xu, 2022. "A medium-entropy transition metal oxide cathode for high-capacity lithium metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    5. Friedrich-W. Wellmer, 2022. "What we have learned from the past and how we should look forward," Mineral Economics, Springer;Raw Materials Group (RMG);Luleå University of Technology, vol. 35(3), pages 765-795, December.

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