Parasitic structure defect blights sustainability of cobalt-free single crystalline cathodes

Lei Yu, Alvin Dai, Tao Zhou, Weiyuan Huang, Jing Wang, Tianyi Li, Xinyou He, Lu Ma, Xianghui Xiao, Mingyuan Ge, Rachid Amine, Steven N. Ehrlich, Xing Ou (), Jianguo Wen (), Tongchao Liu () and Khalil Amine ()
Additional contact information
Lei Yu: Argonne National Laboratory
Alvin Dai: Argonne National Laboratory
Tao Zhou: Argonne National Laboratory
Weiyuan Huang: Argonne National Laboratory
Jing Wang: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Xinyou He: Central South University
Lu Ma: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Rachid Amine: Argonne National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Xing Ou: Central South University
Jianguo Wen: Argonne National Laboratory
Tongchao Liu: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Recent efforts to reduce battery costs and enhance sustainability have focused on eliminating Cobalt (Co) from cathode materials. While Co-free designs have shown notable success in polycrystalline cathodes, their impact on single crystalline (SC) cathodes remains less understood due to the significantly extended lithium diffusion pathways and the higher-temperature synthesis involved. Here, we reveal that removing Co from SC cathodes is structurally and electrochemically unfavorable, exhibiting unusual voltage fade behavior. Using multiscale diffraction and imaging techniques, we identify lithium-rich nanodomains (LRNDs) as a heterogeneous phase within the layered structure of Co-free SC cathodes. These LRNDs act as critical tipping points, inducing significant chemo-mechanical lattice strain and irreversible structural degradation, which exacerbates the voltage and capacity loss in electrochemical performance. Our findings highlight the considerable challenges of developing Co-free SC cathodes compared to polycrystalline ones and emphasize the need for new strategies to balance the interplay between cost, sustainability, and performance.

Date: 2025
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DOI: 10.1038/s41467-024-55235-5

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