Unraveling the origin of air-stability in single-crystalline layered oxide positive electrode materials

Lei Yu, Jing Wang, Tao Zhou, Weiyuan Huang, Tianyi Li, Lu Ma, Xianghui Xiao, Seoung-Bum Son, Steven N. Ehrlich, Jianguo Wen (), Khalil Amine () and Tongchao Liu ()
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Lei Yu: Argonne National Laboratory
Jing Wang: Argonne National Laboratory
Tao Zhou: Argonne National Laboratory
Weiyuan Huang: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Lu Ma: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Seoung-Bum Son: Argonne National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Jianguo Wen: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory
Tongchao Liu: Argonne National Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Single-crystalline Ni-rich layered oxides present compelling advantages over conventional polycrystalline counterparts toward large-scale applications, including enhanced mechanical stability and higher energy density. Nevertheless, the deleterious effects of air exposure, which is inevitable in industrial processing, on their structure and electrochemical performance remain poorly understood. Herein, we reveal that air exposure is more detrimental to the electrochemical performance of single-crystalline layered oxide positive electrodes than polycrystalline counterparts. It is found that air-induced surface structural distortions are primarily responsible for the electrochemical performance decay of single-crystalline samples rather than the generally believed surface residual lithium. Leveraging multiscale diffraction and imaging techniques, we identify an undesirable structural transition to a metastable O1* phase, which introduces substantial lattice defects and localized strain concentrations within the layered structure. These adverse structural evolutions compromise structural integrity and promote crack initiation during electrochemical cycling, ultimately accelerating capacity fade. Our findings provide critical insights into the air-induced degradation mechanisms and emphasize the urgent need for developing effective stabilization strategies to facilitate the commercial implementation of single-crystalline Ni-rich positive electrodes.

Date: 2025
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DOI: 10.1038/s41467-025-61304-0

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