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

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 and Lianzhou Wang ()
Additional contact information
Xiaobo Zhu: The University of Queensland
Tobias U. Schülli: The University of Queensland
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
Zhenxiang Cheng: University of Wollongong, Squires Way
Yi Du: University of Wollongong, Squires Way
Lianzhou Wang: The University of Queensland

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-28963-9

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