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LiMnO2 cathode stabilized by interfacial orbital ordering for sustainable lithium-ion batteries

Author

Listed:
  • Xiaohui Zhu

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Fanqi Meng

    (Chinese Academy of Sciences
    Songshan Lake Materials Laboratory
    University of Chinese Academy of Sciences)

  • Qinghua Zhang

    (Chinese Academy of Sciences
    Songshan Lake Materials Laboratory
    University of Chinese Academy of Sciences)

  • Liang Xue

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • He Zhu

    (City University of Hong Kong)

  • Si Lan

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Qi Liu

    (City University of Hong Kong)

  • Jing Zhao

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Yuhang Zhuang

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Qiubo Guo

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Bo Liu

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

  • Lin Gu

    (Chinese Academy of Sciences
    Songshan Lake Materials Laboratory
    University of Chinese Academy of Sciences)

  • Xia Lu

    (Sun Yat-Sen University)

  • Yang Ren

    (Argonne National Laboratory)

  • Hui Xia

    (Nanjing University of Science and Technology
    Nanjing University of Science and Technology)

Abstract

Global lithium-ion battery deployments stand poised to grow substantially in the coming years, but it will be necessary to include sustainability considerations in the design of electrode materials. The current cathode chemistry relies heavily on cobalt, which, due to its scarcity and the environmental abuse and violation of human rights during its mining, must be replaced by abundant and environmentally friendly elements such as redox-active manganese. LiMnO2 is a strong contender for sustainable cathodes but cycles poorly because the Jahn–Teller distorted Mn3+ ions destabilize the lattice framework. Here, we report a LiMnO2 cathode design with interwoven spinel and layered domains. At the interface between these two domains, the Mn dz2 orbitals are oriented perpendicular to each other, giving rise to interfacial orbital ordering, which suppresses the otherwise cooperative Jahn–Teller distortion and Mn dissolution. As a result, the heterostructured cathode delivers enhanced structural and electrochemical cycling stability. This work provides a new strategy for interface engineering, possibly stimulating more research on Mn-rich cathode materials for sustainable lithium-ion batteries.

Suggested Citation

  • Xiaohui Zhu & Fanqi Meng & Qinghua Zhang & Liang Xue & He Zhu & Si Lan & Qi Liu & Jing Zhao & Yuhang Zhuang & Qiubo Guo & Bo Liu & Lin Gu & Xia Lu & Yang Ren & Hui Xia, 2021. "LiMnO2 cathode stabilized by interfacial orbital ordering for sustainable lithium-ion batteries," Nature Sustainability, Nature, vol. 4(5), pages 392-401, May.
  • Handle: RePEc:nat:natsus:v:4:y:2021:i:5:d:10.1038_s41893-020-00660-9
    DOI: 10.1038/s41893-020-00660-9
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    Cited by:

    1. Shuo Sun & Zhen Han & Wei Liu & Qiuying Xia & Liang Xue & Xincheng Lei & Teng Zhai & Dong Su & Hui Xia, 2023. "Lattice pinning in MoO3 via coherent interface with stabilized Li+ intercalation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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