journal article·2023-10Open access

Boosting reversible anionic redox reaction with Li/Cu dual honeycomb centers

Xiaohui Rong, Dongdong Xiao, Qinghao Li, Yaoshen Niu, Feixiang Ding, Xueyan Hou, Qiyu Wang, Juping Xu, Chenglong Zhao, Dong Zhou, Ruijuan Xiao, Xiqian Yu, Wen Yin, Lin Gu, Hong Li, Xuejie Huang, Liquan Chen, Yong-Sheng Hu

eScience· Volume 3· Issue 5

Abstract

The anionic redox reaction (ARR) is a promising charge contributor to improve the reversible capacity of layered-oxide cathodes for Na-ion batteries; however, some practical bottlenecks still need to be eliminated, including a low capacity retention, large voltage hysteresis, and low rate capability. Herein, we proposed a high-Na content honeycomb-ordered cathode, P2-Na5/6[Li1/6Cu1/6Mn2/3]O2 (P2-NLCMO), with combined cationic/anionic redox. Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry. In addition, advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers, achieving fully active Cu3+/Cu2+ redox and stabilized ARR with interactively suppressed local distortion. With a meticulously regulated charge/discharge protocol, both the cycling and rate capability of P2-NLCMO were significantly improved, demonstrating reasonable capacity and eliminating voltage hysteresis. Overall, this work contributes a well-defined layered oxide cathode with combined cationic/anionic redox towards rational designing advanced Na-ion batteries.
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OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Supercapacitor Materials and Fabrication

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