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Nature Energy · 2024 ·Vol. 9 ·期 3 ·345-356 · IF 49.7

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

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 x Co y Mn 1− x − y O 2 ( 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.

研究领域: 材料科学 · 电化学 · 电池技术
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