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

Zhao, Chen; Wang, Chuanwei; Liu, Xiang; Hwang, Inhui; Li, Tianyi; Zhou, Xinwei; Diao, Jiecheng; Deng, Junjing; Qin, Yan; Yang, Zhenzhen; Wang, Guanyi; Xu, Wenqian; Sun, Chengjun; Wu, Longlong; Cha, Wonsuk; Robinson, Ian; Harder, Ross; Jiang, Yi; Bicer, Tekin; Li, Jun-Tao; Lu, Wenquan; Li, Luxi; Liu, Yuzi; Sun, Shi-Gang; Xu, Gui-Liang; Amine, Khalil

doi:10.1038/s41560-024-01465-2

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

Journal Article · 28 February 2024 · Nature Energy

DOI: https://doi.org/10.1038/s41560-024-01465-2 · OSTI ID:2484299

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^[2]; Liu, Xiang ^[1];

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^[1]; Zhou, Xinwei ^[3]; Diao, Jiecheng ^[4];

^[1]; Qin, Yan ^[1]; Yang, Zhenzhen ^[1]; Wang, Guanyi ^[3];

^[1]; Sun, Chengjun ^[1];

^[5]; Cha, Wonsuk ^[1];

^[6]; Harder, Ross ^[1];

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^[1]; Li, Jun-Tao ^[2] more »

Argonne National Laboratory (ANL), Argonne, IL (United States)
Xiamen University (China)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Univ. College London (United Kingdom); ShanghaiTech Univ. (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Univ. College London (United Kingdom); Brookhaven National Laboratory (BNL), Upton, NY (United States)

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 LiNi_xCo_yMn_1-x-yO₂ (x ≥ 0.9) cathodes via an oriented attachment-driven reaction between Wadsley-Roth phase-based oxides and the layered-oxide cathodes. Further, 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. Layered Ni-rich oxide cathodes are susceptible to challenges with surface reconstruction and strain propagation, limiting their cyclability. The authors propose a solution involving oriented attachment-driven reactions, utilizing Wadsley-Roth nanocrystals and layered oxide to induce an epitaxial entropy-assisted coating, effectively addressing these issues.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2484299

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 3 Vol. 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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