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 HuangTao Zhou, Ming Du, Zonghai Chen, Shi Gang Sun, Maria K.Y. Chan, Wanli Yang*, Minggao Ouyang*, Khalil Amine*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

15 Scopus citations


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.

Original languageEnglish (US)
Pages (from-to)808-817
Number of pages10
JournalNature Energy
Issue number9
StatePublished - Sep 2022
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology


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