Three-dimensional atomic-scale observation of structural evolution of cathode material in a working all-solid-state battery

Yue Gong, Yuyang Chen, Qinghua Zhang, Fanqi Meng, Jin-An Shi, Xinyu Liu, Xiaozhi Liu, Jienan Zhang, Hao Wang, Jiangyong Wang, Qian Yu (), Ze Zhang, Qiang Xu, Ruijuan Xiao, Yong-Sheng Hu, Lin Gu (), Hong Li (), Xuejie Huang and Liquan Chen
Additional contact information
Yue Gong: Chinese Academy of Sciences
Yuyang Chen: Chinese Academy of Sciences
Qinghua Zhang: Chinese Academy of Sciences
Fanqi Meng: Chinese Academy of Sciences
Jin-An Shi: Chinese Academy of Sciences
Xinyu Liu: Chinese Academy of Sciences
Xiaozhi Liu: Chinese Academy of Sciences
Jienan Zhang: Chinese Academy of Sciences
Hao Wang: Chinese Academy of Sciences
Jiangyong Wang: Shantou University, Shantou
Qian Yu: Zhejiang University
Ze Zhang: Zhejiang University
Qiang Xu: DENSsolutions
Ruijuan Xiao: Chinese Academy of Sciences
Yong-Sheng Hu: Chinese Academy of Sciences
Lin Gu: Chinese Academy of Sciences
Hong Li: Chinese Academy of Sciences
Xuejie Huang: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: Abstract Most technologically important electrode materials for lithium-ion batteries are essentially lithium ions plus a transition-metal oxide framework. However, their atomic and electronic structure evolution during electrochemical cycling remains poorly understood. Here we report the in situ observation of the three-dimensional structural evolution of the transition-metal oxide framework in an all-solid-state battery. The in situ studies LiNi0.5Mn1.5O4 from various zone axes reveal the evolution of both atomic and electronic structures during delithiation, which is found due to the migration of oxygen and transition-metal ions. Ordered to disordered structural transition proceeds along the , , directions and inhomogeneous structural evolution along the direction. Uneven extraction of lithium ions leads to localized migration of transition-metal ions and formation of antiphase boundaries. Dislocations facilitate transition-metal ions migration as well. Theoretical calculations suggest that doping of lower valence-state cations effectively stabilize the structure during delithiation and inhibit the formation of boundaries.

Date: 2018
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DOI: 10.1038/s41467-018-05833-x

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