Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V

Jie-Nan Zhang, Qinghao Li, Chuying Ouyang, Xiqian Yu (), Mingyuan Ge, Xiaojing Huang, Enyuan Hu, Chao Ma, Shaofeng Li, Ruijuan Xiao, Wanli Yang, Yong Chu, Yijin Liu (), Huigen Yu, Xiao-Qing Yang, Xuejie Huang, Liquan Chen and Hong Li ()
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Jie-Nan Zhang: Chinese Academy of Sciences
Qinghao Li: Chinese Academy of Sciences
Chuying Ouyang: Jiangxi Normal University
Xiqian Yu: Chinese Academy of Sciences
Mingyuan Ge: Brookhaven National Laboratory
Xiaojing Huang: Brookhaven National Laboratory
Enyuan Hu: Brookhaven National Laboratory
Chao Ma: Hunan University
Shaofeng Li: SLAC National Accelerator Laboratory
Ruijuan Xiao: Chinese Academy of Sciences
Wanli Yang: Lawrence Berkeley National Laboratory
Yong Chu: Brookhaven National Laboratory
Yijin Liu: SLAC National Accelerator Laboratory
Huigen Yu: Beijing WeLion New Energy Technology
Xiao-Qing Yang: Brookhaven National Laboratory
Xuejie Huang: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences
Hong Li: Chinese Academy of Sciences

Nature Energy, 2019, vol. 4, issue 7, 594-603

Abstract: Abstract LiCoO2 is a dominant cathode material for lithium-ion (Li-ion) batteries due to its high volumetric energy density, which could potentially be further improved by charging to high voltages. However, practical adoption of high-voltage charging is hindered by LiCoO2’s structural instability at the deeply delithiated state and the associated safety concerns. Here, we achieve stable cycling of LiCoO2 at 4.6 V (versus Li/Li+) through trace Ti–Mg–Al co-doping. Using state-of-the-art synchrotron X-ray imaging and spectroscopic techniques, we report the incorporation of Mg and Al into the LiCoO2 lattice, which inhibits the undesired phase transition at voltages above 4.5 V. We also show that, even in trace amounts, Ti segregates significantly at grain boundaries and on the surface, modifying the microstructure of the particles while stabilizing the surface oxygen at high voltages. These dopants contribute through different mechanisms and synergistically promote the cycle stability of LiCoO2 at 4.6 V.

Date: 2019
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DOI: 10.1038/s41560-019-0409-z

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