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

Nature Communications - Tập 12 Số 1
Haifeng Yu1, Yueqiang Cao2, Long Chen1, Yanjie Hu1, Xuezhi Duan2, Sheng Dai3, Chunzhong Li1, Hao Jiang1
1Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai, China
2State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, China
3Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China

Tóm tắt

AbstractCritical 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.

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