Rational design of mechanically robust Ni-rich cathode materials via concentration gradient strategy

Tongchao Liu, Lei Yu, Jun Lu (), Tao Zhou, Xiaojing Huang, Zhonghou Cai, Alvin Dai, Jihyeon Gim, Yang Ren, Xianghui Xiao, Martin V. Holt, Yong S. Chu, Ilke Arslan, Jianguo Wen () and Khalil Amine ()
Additional contact information
Tongchao Liu: Argonne National Laboratory
Lei Yu: Argonne National Laboratory
Jun Lu: Argonne National Laboratory
Tao Zhou: Argonne National Laboratory
Xiaojing Huang: Brookhaven National Laboratory
Zhonghou Cai: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Jihyeon Gim: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Martin V. Holt: Argonne National Laboratory
Yong S. Chu: Brookhaven National Laboratory
Ilke Arslan: Argonne National Laboratory
Jianguo Wen: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Mechanical integrity issues such as particle cracking are considered one of the leading causes of structural deterioration and limited long-term cycle stability for Ni-rich cathode materials of Li-ion batteries. Indeed, the detrimental effects generated from the crack formation are not yet entirely addressed. Here, applying physicochemical and electrochemical ex situ and in situ characterizations, the effect of Co and Mn on the mechanical properties of the Ni-rich material are thoroughly investigated. As a result, we successfully mitigate the particle cracking issue in Ni-rich cathodes via rational concentration gradient design without sacrificing the electrode capacity. Our result reveals that the Co-enriched surface design in Ni-rich particles benefits from its low stiffness, which can effectively suppress the formation of particle cracking. Meanwhile, the Mn-enriched core limits internal expansion and improve structural integrity. The concentration gradient design also promotes morphological stability and cycling performances in Li metal coin cell configuration.

Date: 2021
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DOI: 10.1038/s41467-021-26290-z

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