Real-space measurement of orbital electron populations for Li1-xCoO2

Tongtong Shang, Dongdong Xiao, Fanqi Meng, Xiaohui Rong, Ang Gao, Ting Lin, Zhexin Tang, Xiaozhi Liu, Xinyan Li, Qinghua Zhang, Yuren Wen, Ruijuan Xiao, Xuefeng Wang, Dong Su, Yong-Sheng Hu, Hong Li, Qian Yu, Ze Zhang, Vaclav Petricek, Lijun Wu (), Lin Gu (), Jian-Min Zuo, Yimei Zhu, Ce-Wen Nan and Jing Zhu
Additional contact information
Tongtong Shang: Chinese Academy of Sciences
Dongdong Xiao: Chinese Academy of Sciences
Fanqi Meng: Tsinghua University
Xiaohui Rong: Chinese Academy of Sciences
Ang Gao: Chinese Academy of Sciences
Ting Lin: Chinese Academy of Sciences
Zhexin Tang: Chinese Academy of Sciences
Xiaozhi Liu: Chinese Academy of Sciences
Xinyan Li: Chinese Academy of Sciences
Qinghua Zhang: Chinese Academy of Sciences
Yuren Wen: University of Science and Technology Beijing
Ruijuan Xiao: Chinese Academy of Sciences
Xuefeng Wang: Chinese Academy of Sciences
Dong Su: Chinese Academy of Sciences
Yong-Sheng Hu: Chinese Academy of Sciences
Hong Li: Chinese Academy of Sciences
Qian Yu: Zhejiang University
Ze Zhang: Zhejiang University
Vaclav Petricek: Academy of Sciences of the Czech Republic
Lijun Wu: Brookhaven National Laboratory
Lin Gu: Chinese Academy of Sciences
Jian-Min Zuo: University of Illinois at Urbana Champaign
Yimei Zhu: Brookhaven National Laboratory
Ce-Wen Nan: Tsinghua University
Jing Zhu: Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract The operation of lithium-ion batteries involves electron removal from and filling into the redox orbitals of cathode materials, experimentally probing the orbital electron population thus is highly desirable to resolve the redox processes and charge compensation mechanism. Here, we combine quantitative convergent-beam electron diffraction with high-energy synchrotron powder X-ray diffraction to quantify the orbital populations of Co and O in the archetypal cathode material LiCoO2. The results indicate that removing Li ions from LiCoO2 decreases Co t2g orbital population, and the intensified covalency of Co–O bond upon delithiation enables charge transfer from O 2p orbital to Co eg orbital, leading to increased Co eg orbital population and oxygen oxidation. Theoretical calculations verify these experimental findings, which not only provide an intuitive picture of the redox reaction process in real space, but also offer a guidance for designing high-capacity electrodes by mediating the covalency of the TM–O interactions.

Date: 2022
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DOI: 10.1038/s41467-022-33595-0

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