Suppressing strain propagation in ultrahigh-Ni cathodes during fast charging via epitaxial entropy-assisted coating

Chen Zhao, Chuanwei Wang, Xiang Liu, Inhui Hwang, Tianyi Li, Xinwei Zhou, Jiecheng Diao, Junjing Deng, Yan Qin, Zhenzhen Yang, Guanyi Wang, Wenqian Xu, Chengjun Sun, Longlong Wu, Wonsuk Cha, Ian Robinson, Ross Harder, Yi Jiang, Tekin Bicer, Jun-Tao Li, Wenquan Lu, Luxi Li (), Yuzi Liu (), Shi-Gang Sun, Gui-Liang Xu () and Khalil Amine ()
Additional contact information
Chen Zhao: Argonne National Laboratory
Chuanwei Wang: Xiamen University
Xiang Liu: Argonne National Laboratory
Inhui Hwang: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Xinwei Zhou: Argonne National Laboratory
Jiecheng Diao: University College London
Junjing Deng: Argonne National Laboratory
Yan Qin: Argonne National Laboratory
Zhenzhen Yang: Argonne National Laboratory
Guanyi Wang: Argonne National Laboratory
Wenqian Xu: Argonne National Laboratory
Chengjun Sun: Argonne National Laboratory
Longlong Wu: Brookhaven National Laboratory
Wonsuk Cha: Argonne National Laboratory
Ian Robinson: University College London
Ross Harder: Argonne National Laboratory
Yi Jiang: Argonne National Laboratory
Tekin Bicer: Argonne National Laboratory
Jun-Tao Li: Xiamen University
Wenquan Lu: Argonne National Laboratory
Luxi Li: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
Shi-Gang Sun: Xiamen University
Gui-Liang Xu: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory

Nature Energy, 2024, vol. 9, issue 3, 345-356

Abstract: Abstract Surface reconstruction and the associated severe strain propagation have long been reported as the major cause of cathode failure during fast charging and long-term cycling. Despite tremendous attempts, no known strategies can simultaneously address the electro-chemomechanical instability without sacrificing energy and power density. Here we report an epitaxial entropy-assisted coating strategy for ultrahigh-Ni LiNixCoyMn1−x−yO2 (x ≥ 0.9) cathodes via an oriented attachment-driven reaction between Wadsley–Roth phase-based oxides and the layered-oxide cathodes. The high anti-cracking and anti-corrosion tolerances as well as the fast ionic transport of the entropy-assisted surface effectively improved the fast charging/discharging capability, wide temperature tolerance and thermal stability of the ultrahigh-Ni cathodes. Comprehensive analysis from the primary and secondary particle level to the electrode level using multi-scale in situ synchrotron X-ray probes reveals greatly reduced lattice dislocations, anisotropic lattice strain and oxygen release as well as improved bulk/local structural stability, even when charging beyond the threshold state of charge (75%) of layered cathodes.

Date: 2024
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DOI: 10.1038/s41560-024-01465-2

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