DOE OSTI · 2530426
Kinetically Dormant Ni‐Rich Layered Cathode During High‐Voltage Operation
Abstract
Abstract The degradation of Ni‐rich cathodes during long‐term operation at high voltage has garnered significant attention from both academia and industry. Despite many post‐mortem qualitative structural analyses, precise quantification of their individual and coupling contributions to the overall capacity degradation remains challenging. Here, by leveraging multiscale synchrotron X‐ray probes, electron microscopy, and post‐galvanostatic intermittent titration technique, the thermodynamically irreversible and kinetically reversible capacity loss is successfully deconvoluted in a polycrystalline LiNi 0.83 Mn 0.1 Co 0.07 O 2 cathode during long‐term charge/discharge cycling in full cell configuration. Contradicting the dramatic capacity loss, the layered structure remains highly alive even after 1000 cycles at 4.6 V while undergoing a three‐order of magnitude reduction in the mass transfer kinetics, leading to almost fully recoverable capacity under kinetic‐free conditions. Such kinetic dormant behavior after cycling is not simply ascribed to poor chemical diffusion by reconstructed cathode surface but highly synchronizes with the lattice strain evolution stemming from the structural heterogeneity between deeply delithiated layered and degraded rock‐salt phases at high voltage. These findings deepen the degradation mechanism of high‐voltage cathodes to achieve long‐cycling and fast‐charging performance.
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Cai, Jiyu [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA], Zhou, Xinwei [Center for Nanoscale Materials Argonne National Laboratory Lemont IL 60439 USA], Li, Luxi [Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA], Yang, Zhenzhen [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA], Huang, Xingkang [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA], Li, Jiantao [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA], Wang, Guanyi [Center for Nanoscale Materials Argonne National Laboratory Lemont IL 60439 USA], Zhu, Qijia [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA], Li, Tianyi [Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA], Sun, Cheng‐Jun [Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA], Zhuo, Zengqing [Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA], Suzana, Ana [Condensed Matter Physics and Materials Science Department Brookhaven National Laboratory Upton NY 11973 USA], Bai, Jianming [Condensed Matter Physics and Materials Science Department Brookhaven National Laboratory Upton NY 11973 USA], Gudavalli, Ganesh [Charge CCCV (C4V) Center of Excellence Binghamton University Vestal NY 13850 USA], Karami, Niloofar [Charge CCCV (C4V) Center of Excellence Binghamton University Vestal NY 13850 USA], Chernova, Natasha A. [Charge CCCV (C4V) Center of Excellence Binghamton University Vestal NY 13850 USA], Upreti, Shailesh [Charge CCCV (C4V) Center of Excellence Binghamton University Vestal NY 13850 USA], Prevel, Brad [Primet Precision Materials Ithaca NY 14850 USA], Yang, Wanli [Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA], Liu, Yuzi [Center for Nanoscale Materials Argonne National Laboratory Lemont IL 60439 USA], Xu, Wenqian [Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA], Chen, Yanbin [Beijing Easpring Material Technology Co. Ltd. Beijing 100160 China], Song, Shunlin [Beijing Easpring Material Technology Co. Ltd. Beijing 100160 China], Zhang, Xuequan [Beijing Easpring Material Technology Co. Ltd. Beijing 100160 China], Wang, Li [Institute of Nuclear and New Energy Technology Tsinghua University Beijing 100084 China], He, Xiangming [Institute of Nuclear and New Energy Technology Tsinghua University Beijing 100084 China], Wang, Feng [Applied Materials Division Argonne National Laboratory Lemont IL 60439 USA], Xu, Gui‐Liang [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA] (ORCID:000000019969883X), Chen, Zonghai [Chemical Sciences and Engineering Division Argonne National Laboratory Lemont IL 60439 USA]. 2025-03-03. Kinetically Dormant Ni‐Rich Layered Cathode During High‐Voltage Operation. https://doi.org/10.1002/adma.202419253
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