Origin and regulation of oxygen redox instability in high-voltage battery cathodes

Xiang Liu, Gui-Liang Xu (), Venkata Surya Chaitanya Kolluru, Chen Zhao, Qingtian Li, Xinwei Zhou, Yuzi Liu, Liang Yin, Zengqing Zhuo, Amine Daali, Jing-Jing Fan, Wenjun Liu, Yang Ren, Wenqian Xu, Junjing Deng, Inhui Hwang, Dongsheng Ren, Xuning Feng, Chengjun Sun, Ling Huang, Tao Zhou, Ming Du, Zonghai Chen, Shi-Gang Sun, Maria K. Y. Chan, Wanli Yang (), Minggao Ouyang () and Khalil Amine ()
Additional contact information
Xiang Liu: Argonne National Laboratory
Gui-Liang Xu: Argonne National Laboratory
Venkata Surya Chaitanya Kolluru: Argonne National Laboratory
Chen Zhao: Argonne National Laboratory
Qingtian Li: Lawrence Berkeley National Laboratory
Xinwei Zhou: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
Liang Yin: Argonne National Laboratory
Zengqing Zhuo: Lawrence Berkeley National Laboratory
Amine Daali: Argonne National Laboratory
Jing-Jing Fan: Xiamen University
Wenjun Liu: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Wenqian Xu: Argonne National Laboratory
Junjing Deng: Argonne National Laboratory
Inhui Hwang: Argonne National Laboratory
Dongsheng Ren: Tsinghua University
Xuning Feng: Tsinghua University
Chengjun Sun: Argonne National Laboratory
Ling Huang: Xiamen University
Tao Zhou: Argonne National Laboratory
Ming Du: Argonne National Laboratory
Zonghai Chen: Argonne National Laboratory
Shi-Gang Sun: Xiamen University
Maria K. Y. Chan: Argonne National Laboratory
Wanli Yang: Lawrence Berkeley National Laboratory
Minggao Ouyang: Tsinghua University
Khalil Amine: Argonne National Laboratory

Nature Energy, 2022, vol. 7, issue 9, 808-817

Abstract: Abstract Oxygen redox at high voltage has emerged as a transformative paradigm for high-energy battery cathodes such as layered transition-metal oxides by offering extra capacity beyond conventional transition-metal redox. However, these cathodes suffer from voltage hysteresis, voltage fade and capacity drop upon cycling. Single-crystalline cathodes have recently shown some improvements, but these challenges remain. Here we reveal the fundamental origin of oxygen redox instability to be from the domain boundaries that are present in single-crystalline cathode particles. By investigating single-crystalline cathodes with different domain boundaries structures, we show that the elimination of domain boundaries enhances the reversible lattice oxygen redox while inhibiting the irreversible oxygen release. This leads to significantly suppressed structural degradation and improved mechanical integrity during battery cycling and abuse heating. The robust oxygen redox enabled through domain boundary control provides practical opportunities towards high-energy, long-cycling, safe batteries.

Date: 2022
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DOI: 10.1038/s41560-022-01036-3

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