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Epitaxial growth of an atom-thin layer on a LiNi0.5Mn1.5O4 cathode for stable Li-ion battery cycling

Author

Listed:
  • Xiaobo Zhu

    (The University of Queensland
    Changsha University of Science and Technology)

  • Tobias U. Schülli

    (The University of Queensland
    ESRF—The European Synchrotron)

  • Xiaowei Yang

    (Ion and Electron Beams (Dalian University of Technology), Ministry of Education)

  • Tongen Lin

    (The University of Queensland)

  • Yuxiang Hu

    (The University of Queensland)

  • Ningyan Cheng

    (University of Wollongong, Squires Way)

  • Hiroki Fujii

    (National Institute for Materials Science)

  • Kiyoshi Ozawa

    (National Institute for Materials Science)

  • Bruce Cowie

    (Australian Synchrotron)

  • Qinfen Gu

    (Australian Synchrotron)

  • Si Zhou

    (Ion and Electron Beams (Dalian University of Technology), Ministry of Education
    University of Wollongong, Squires Way)

  • Zhenxiang Cheng

    (University of Wollongong, Squires Way)

  • Yi Du

    (University of Wollongong, Squires Way)

  • Lianzhou Wang

    (The University of Queensland)

Abstract

Transition metal dissolution in cathode active material for Li-based batteries is a critical aspect that limits the cycle life of these devices. Although several approaches have been proposed to tackle this issue, this detrimental process is not yet overcome. Here, benefitting from the knowledge developed in the semiconductor research field, we apply an epitaxial method to construct an atomic wetting layer of LaTMO3 (TM = Ni, Mn) on a LiNi0.5Mn1.5O4 cathode material. Experimental measurements and theoretical analyses confirm a Stranski–Krastanov growth, where the strained wetting layer forms under thermodynamic equilibrium, and it is self-limited to monoatomic thickness due to the competition between the surface energy and the elastic energy. Being atomically thin and crystallographically connected to the spinel host lattices, the LaTMO3 wetting layer offers long-term suppression of the transition metal dissolution from the cathode without impacting its dynamics. As a result, the epitaxially-engineered cathode material enables improved cycling stability (a capacity retention of about 77% after 1000 cycles at 290 mA g−1) when tested in combination with a graphitic carbon anode and a LiPF6-based non-aqueous electrolyte solution.

Suggested Citation

  • Xiaobo Zhu & Tobias U. Schülli & Xiaowei Yang & Tongen Lin & Yuxiang Hu & Ningyan Cheng & Hiroki Fujii & Kiyoshi Ozawa & Bruce Cowie & Qinfen Gu & Si Zhou & Zhenxiang Cheng & Yi Du & Lianzhou Wang, 2022. "Epitaxial growth of an atom-thin layer on a LiNi0.5Mn1.5O4 cathode for stable Li-ion battery cycling," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28963-9
    DOI: 10.1038/s41467-022-28963-9
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    References listed on IDEAS

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    1. Jianhui Wang & Yuki Yamada & Keitaro Sodeyama & Ching Hua Chiang & Yoshitaka Tateyama & Atsuo Yamada, 2016. "Superconcentrated electrolytes for a high-voltage lithium-ion battery," Nature Communications, Nature, vol. 7(1), pages 1-9, November.
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    1. Isaac Martens & Nikita Vostrov & Marta Mirolo & Steven J. Leake & Edoardo Zatterin & Xiaobo Zhu & Lianzhou Wang & Jakub Drnec & Marie-Ingrid Richard & Tobias U. Schulli, 2023. "Defects and nanostrain gradients control phase transition mechanisms in single crystal high-voltage lithium spinel," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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