Inhibition of oxygen dimerization by local symmetry tuning in Li-rich layered oxides for improved stability

Fanghua Ning, Biao Li, Jin Song, Yuxuan Zuo, Huaifang Shang, Zimeng Zhao, Zhen Yu, Wangsheng Chu (), Kun Zhang, Guang Feng, Xiayan Wang () and Dingguo Xia ()
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Fanghua Ning: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Biao Li: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Jin Song: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Yuxuan Zuo: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Huaifang Shang: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Zimeng Zhao: Beijing University of Technology
Zhen Yu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wangsheng Chu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Kun Zhang: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Guang Feng: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University
Xiayan Wang: Beijing University of Technology
Dingguo Xia: Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, College of Engineering, Peking University

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract Li-rich layered oxide cathode materials show high capacities in lithium-ion batteries owing to the contribution of the oxygen redox reaction. However, structural accommodation of this reaction usually results in O–O dimerization, leading to oxygen release and poor electrochemical performance. In this study, we propose a new structural response mechanism inhibiting O–O dimerization for the oxygen redox reaction by tuning the local symmetry around the oxygen ions. Compared with regular Li2RuO3, the structural response of the as-prepared local-symmetry-tuned Li2RuO3 to the oxygen redox reaction involves the telescopic O–Ru–O configuration rather than O–O dimerization, which inhibits oxygen release, enabling significantly enhanced cycling stability and negligible voltage decay. This discovery of the new structural response mechanism for the oxygen redox reaction will provide a new scope for the strategy of enhancing the anionic redox stability, paving unexplored pathways toward further development of high capacity Li-rich layered oxides.

Date: 2020
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DOI: 10.1038/s41467-020-18423-7

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