Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage

Fang Zhang, Shuaifeng Lou, Shuang Li, Zhenjiang Yu, Qingsong Liu, Alvin Dai, Chuntian Cao, Michael F. Toney, Mingyuan Ge, Xianghui Xiao, Wah-Keat Lee, Yudong Yao, Junjing Deng, Tongchao Liu, Yiping Tang, Geping Yin, Jun Lu (), Dong Su () and Jiajun Wang ()
Additional contact information
Fang Zhang: School of Chemistry and Chemical Engineering, Harbin Institute of Technology
Shuaifeng Lou: School of Chemistry and Chemical Engineering, Harbin Institute of Technology
Shuang Li: Brookhaven National Laboratory
Zhenjiang Yu: School of Chemistry and Chemical Engineering, Harbin Institute of Technology
Qingsong Liu: School of Chemistry and Chemical Engineering, Harbin Institute of Technology
Alvin Dai: Argonne National Laboratory
Chuntian Cao: SLAC National Accelerator Laboratory
Michael F. Toney: SLAC National Accelerator Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Wah-Keat Lee: Brookhaven National Laboratory
Yudong Yao: Argonne National Laboratory
Junjing Deng: Argonne National Laboratory
Tongchao Liu: Argonne National Laboratory
Yiping Tang: Zhejiang University of Technology
Geping Yin: School of Chemistry and Chemical Engineering, Harbin Institute of Technology
Jun Lu: Argonne National Laboratory
Dong Su: Institute of Physics, Chinese Academy of Sciences
Jiajun Wang: School of Chemistry and Chemical Engineering, Harbin Institute of Technology

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract Single-crystal cathode materials for lithium-ion batteries have attracted increasing interest in providing greater capacity retention than their polycrystalline counterparts. However, after being cycled at high voltages, these single-crystal materials exhibit severe structural instability and capacity fade. Understanding how the surface structural changes determine the performance degradation over cycling is crucial, but remains elusive. Here, we investigate the correlation of the surface structure, internal strain, and capacity deterioration by using operando X-ray spectroscopy imaging and nano-tomography. We directly observe a close correlation between surface chemistry and phase distribution from homogeneity to heterogeneity, which induces heterogeneous internal strain within the particle and the resulting structural/performance degradation during cycling. We also discover that surface chemistry can significantly enhance the cyclic performance. Our modified process effectively regulates the performance fade issue of single-crystal cathode and provides new insights for improved design of high-capacity battery materials.

Date: 2020
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DOI: 10.1038/s41467-020-16824-2

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