Additive engineering for robust interphases to stabilize high-Ni layered structures at ultra-high voltage of 4.8 V

Sha Tan, Zulipiya Shadike, Jizhou Li, Xuelong Wang, Yang Yang, Ruoqian Lin, Arthur Cresce, Jiangtao Hu, Adrian Hunt, Iradwikanari Waluyo, Lu Ma, Federico Monaco, Peter Cloetens, Jie Xiao, Yijin Liu (), Xiao-Qing Yang (), Kang Xu () and Enyuan Hu ()
Additional contact information
Sha Tan: Brookhaven National Laboratory
Zulipiya Shadike: Brookhaven National Laboratory
Jizhou Li: SLAC National Accelerator Laboratory
Xuelong Wang: Brookhaven National Laboratory
Yang Yang: Brookhaven National Laboratory
Ruoqian Lin: Brookhaven National Laboratory
Arthur Cresce: US Army Research Laboratory
Jiangtao Hu: Pacific Northwest National Laboratory
Adrian Hunt: Brookhaven National Laboratory
Iradwikanari Waluyo: Brookhaven National Laboratory
Lu Ma: Brookhaven National Laboratory
Federico Monaco: European Synchrotron Radiation Facility
Peter Cloetens: European Synchrotron Radiation Facility
Jie Xiao: Pacific Northwest National Laboratory
Yijin Liu: SLAC National Accelerator Laboratory
Xiao-Qing Yang: Brookhaven National Laboratory
Kang Xu: US Army Research Laboratory
Enyuan Hu: Brookhaven National Laboratory

Nature Energy, 2022, vol. 7, issue 6, 484-494

Abstract: Abstract Nickel-rich layered cathode materials promise high energy density for next-generation batteries when coupled with lithium metal anodes. However, the practical capacities accessible are far less than the theoretical values due to their structural instability during cycling, especially when charged at high voltages. Here we demonstrate that stable cycling with an ultra-high cut-off voltage of 4.8 V can be realized by using an appropriate amount of lithium difluorophosphate in a common commercial electrolyte. The Li||LiNi0.76Mn0.14Co0.10O2 cell retains 97% of the initial capacity (235 mAh g–1) after 200 cycles. The cycling stability is ascribed to the robust interphase on the cathode. It is formed by lithium difluorophosphate decomposition, which is facilitated by the catalytic effect of transition metals. The decomposition products (Li3PO4 and LiF) form a protective interphase. This suppresses transition metal dissolution and cathode surface reconstruction. It also facilitates uniform Li distribution within the cathode, effectively mitigating the strain and crack formation.

Date: 2022
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DOI: 10.1038/s41560-022-01020-x

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