Stalling oxygen evolution in high-voltage cathodes by lanthurization

Mingzhi Cai, Yanhao Dong, Miao Xie, Wujie Dong, Chenlong Dong, Peng Dai, Hui Zhang, Xin Wang, Xuzhou Sun, Shaoning Zhang, Moonsu Yoon, Haowei Xu, Yunsong Ge, Ju Li () and Fuqiang Huang ()
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Mingzhi Cai: Peking University
Yanhao Dong: Massachusetts Institute of Technology
Miao Xie: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Wujie Dong: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Chenlong Dong: Tianjin University of Technology
Peng Dai: Xiamen University
Hui Zhang: Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Xin Wang: Zhengzhou University
Xuzhou Sun: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Shaoning Zhang: Shanghai Institute of Ceramics, Chinese Academy of Sciences
Moonsu Yoon: Massachusetts Institute of Technology
Haowei Xu: Massachusetts Institute of Technology
Yunsong Ge: Peking University
Ju Li: Massachusetts Institute of Technology
Fuqiang Huang: Peking University

Nature Energy, 2023, vol. 8, issue 2, 159-168

Abstract: Abstract Coatings and surface passivation are sought to protect high-energy-density cathodes in lithium-ion batteries, which suffer from labile oxygen loss and fast degradations. Here we develop the theory underlying the high-voltage-induced oxygen evolution crisis and report a lanthurizing process to regulate the near-surface structure of energy materials beyond conventional surface doping. Using LiCoO2 as an example and generalizing to Co-lean/free high-energy-density layered cathodes, we demonstrate effective surface passivation, suppressed surface degradation and improved electrochemical performance. High-voltage cycling stability has been greatly enhanced, up to 4.8 V versus Li+/Li, including in practical pouch-type full cells. The superior performance is rooted in the engineered surface architecture and the reliability of the synthesis method. The designed surface phase stalls oxygen evolution reaction at high voltages. It illustrates processing opportunities for surface engineering and coating by high-oxygen-activity passivation, selective chemical alloying and strain engineering using wet chemistry.

Date: 2023
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DOI: 10.1038/s41560-022-01179-3

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