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A Li-rich layered oxide cathode with negligible voltage decay

Dong Luo, He Zhu, Yi Xia, Zijia Yin, Yan Qin, Tianyi Li, Qinghua Zhang, Lin Gu, Yong Peng, Junwei Zhang, Kamila M. Wiaderek, Yalan Huang, Tingting Yang, Yu Tang, Si Lan, Yang Ren (), Wenquan Lu (), Christopher M. Wolverton () and Qi Liu ()
Additional contact information
Dong Luo: City University of Hong Kong
He Zhu: City University of Hong Kong
Yi Xia: Northwestern University
Zijia Yin: City University of Hong Kong
Yan Qin: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Qinghua Zhang: Chinese Academy of Sciences
Lin Gu: Tsinghua University
Yong Peng: Lanzhou University
Junwei Zhang: Lanzhou University
Kamila M. Wiaderek: Argonne National Laboratory
Yalan Huang: City University of Hong Kong
Tingting Yang: City University of Hong Kong
Yu Tang: City University of Hong Kong
Si Lan: City University of Hong Kong
Yang Ren: City University of Hong Kong
Wenquan Lu: Argonne National Laboratory
Christopher M. Wolverton: Northwestern University
Qi Liu: City University of Hong Kong

Nature Energy, 2023, vol. 8, issue 10, 1078-1087

Abstract: Abstract With high capacity at low cost, Li- and Mn-rich (LMR) layered oxides are a promising class of cathodes for next-generation Li-ion batteries. However, substantial voltage decay during cycling, due to the unstable Li2MnO3 honeycomb structure, is still an obstacle to their practical deployment. Here we report a Co-free LMR Li-ion battery cathode with negligible voltage decay. The material has a composite structure consisting of layered LiTMO2 and various stacked Li2MnO3 components, where transition metal (TM) ions that reside in the Li layers of Li2MnO3 form caps to strengthen the stability of the honeycomb structure. This capped-honeycomb structure is persistent after high-voltage cycling and prevents TM migration and oxygen loss as shown by experimental and computational results. This work demonstrates that the long-standing voltage decay problem in LMRs can be effectively mitigated by internally pinning the honeycomb structure, which opens an avenue to developing next-generation high-energy cathode materials.

Date: 2023
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DOI: 10.1038/s41560-023-01289-6

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