Understanding Co roles towards developing Co-free Ni-rich cathodes for rechargeable batteries

Tongchao Liu, Lei Yu, Jiajie Liu, Jun Lu (), Xuanxuan Bi, Alvin Dai, Matthew Li, Maofan Li, Zongxiang Hu, Lu Ma, Duan Luo, Jiaxin Zheng, Tianpin Wu, Yang Ren, Jianguo Wen, Feng Pan () and Khalil Amine ()
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Tongchao Liu: Argonne National Laboratory
Lei Yu: Argonne National Laboratory
Jiajie Liu: Peking University Shenzhen Graduate School
Jun Lu: Argonne National Laboratory
Xuanxuan Bi: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Matthew Li: Argonne National Laboratory
Maofan Li: Peking University Shenzhen Graduate School
Zongxiang Hu: Peking University Shenzhen Graduate School
Lu Ma: Argonne National Laboratory
Duan Luo: Argonne National Laboratory
Jiaxin Zheng: Peking University Shenzhen Graduate School
Tianpin Wu: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Jianguo Wen: Argonne National Laboratory
Feng Pan: Peking University Shenzhen Graduate School
Khalil Amine: Argonne National Laboratory

Nature Energy, 2021, vol. 6, issue 3, 277-286

Abstract: Abstract Current bottlenecks in cobalt (Co) supply have negatively impacted commercial battery production and inspired the development of cathode materials that are less reliant on Co. However, complete Co elimination is prevented by the lack of fundamental understanding of the impact of Co on cathode capacity and structural stability, as well as the lack of effective substitute components in practice. Here we investigate the roles of Co in purposely designed systems that include both Co-rich and Mn-substituted Co-free cathodes. Our results affirmed that Co plays an undeniable role in fast capacity and/or structural degradation, and found that Co is more destructive than Ni at high potentials, which offers unexpected but encouraging perspectives for Co reduction. Moreover, Mn substitution effectively alleviates the destructive effects of Co and enables a high potential functionality. With these fundamental discoveries, we demonstrated a series of LiNiαMnβXγO2 (X = single or multiple dopants) as a promising candidate for Co-free cathodes.

Date: 2021
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DOI: 10.1038/s41560-021-00776-y

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