Authors
Liu, Xiang; Xu, Gui-Liang; Kolluru, Venkata Surya Chaitanya; Zhao, Chen; Li, Qingtian; Zhou, Xinwei; Liu, Yuzi; Yin, Liang; Zhuo, Zengqing; Daali, Amine; Fan, Jingjing; Liu, Wenjun; Ren, Yang; Xu, Wenqian; Deng, Junjing; Hwang, Inhui; Ren, Dongsheng; Feng, Xuning; Sun, Cheng-Jun; Huang, Ling; Zhou, Tao; Du, Ming; Chen, Zonghai; Sun, Shi-Gang; Chan, Maria; Yang, Wanli; Ouyang, Minggao; Amine, Khalil
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 still remain. Here we reveal the fundamental origin of oxygen redox instability to be originated from the domain boundaries that are present in single-crystalline cathode particles. By synthesizing single-crystalline cathodes free of domain boundaries, 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, and safe batteries.