Surface enrichment and diffusion enabling gradient-doping and coating of Ni-rich cathode toward Li-ion batteries

Haifeng Yu, Yueqiang Cao, Long Chen, Yanjie Hu, Xuezhi Duan, Sheng Dai, Chunzhong Li and Hao Jiang ()
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Haifeng Yu: East China University of Science and Technology
Yueqiang Cao: East China University of Science and Technology
Long Chen: East China University of Science and Technology
Yanjie Hu: East China University of Science and Technology
Xuezhi Duan: East China University of Science and Technology
Sheng Dai: East China University of Science and Technology
Chunzhong Li: East China University of Science and Technology
Hao Jiang: East China University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Critical barriers to layered Ni-rich cathode commercialisation include their rapid capacity fading and thermal runaway from crystal disintegration and their interfacial instability. Structure combines surface modification is the ultimate choice to overcome these. Here, a synchronous gradient Al-doped and LiAlO2-coated LiNi0.9Co0.1O2 cathode is designed and prepared by using an oxalate-assisted deposition and subsequent thermally driven diffusion method. Theoretical calculations, in situ X-ray diffraction results and finite-element simulation verify that Al3+ moves to the tetrahedral interstices prior to Ni2+ that eliminates the Li/Ni disorder and internal structure stress. The Li+-conductive LiAlO2 skin prevents electrolyte penetration of the boundaries and reduces side reactions. These help the Ni-rich cathode maintain a 97.4% cycle performance after 100 cycles, and a rapid charging ability of 127.7 mAh g−1 at 20 C. A 3.5-Ah pouch cell with the cathode and graphite anode showed more than a 500-long cycle life with only a 5.6% capacity loss.

Date: 2021
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DOI: 10.1038/s41467-021-24893-0

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