Intralattice-bonded phase-engineered ultrahigh-Ni single-crystalline cathodes suppress strain evolution

Qimeng Zhang, Jing Wang, Youqi Chu, Weiyuan Huang, Xiaojing Huang, Xianghui Xiao, Lu Ma, Tongchao Liu (), Khalil Amine (), Jun Lu () and Chenghao Yang ()
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Qimeng Zhang: South China University of Technology
Jing Wang: Argonne National Laboratory
Youqi Chu: South China University of Technology
Weiyuan Huang: Argonne National Laboratory
Xiaojing Huang: Brookhaven National Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Lu Ma: Brookhaven National Laboratory
Tongchao Liu: Argonne National Laboratory
Khalil Amine: Argonne National Laboratory
Jun Lu: College of Chemical and Biological Engineering Zhejiang University
Chenghao Yang: South China University of Technology

Nature Energy, 2025, vol. 10, issue 8, 1001-1012

Abstract: Abstract Single crystallization remains a debated strategy for advancing Ni-rich cathode materials. While it mitigates particle cracking and improves tap density by eliminating particle boundaries, extended diffusion pathways introduce volumetric and lattice distortions, compromising electrochemical and structural stability. These challenges hinder the commercialization of high-Ni single-crystal cathodes, calling for a reassessment of their viability. Here we report a structural design: intralattice-bonded phase single-crystal LiNi0.92Co0.03Mn0.05O2 (IBP-SC92). This architecture maintains structural integrity while shortening diffusion pathways, resulting in almost zero electrochemical degradation during cycling. The robust structure and fast ion transport mitigate lattice strain, as confirmed by multiscale high-resolution diffraction and imaging techniques, preventing intragranular cracks and irreversible phase transitions. As a result, IBP-SC92 shows outstanding cycling stability, with nearly 100% capacity retention after 100 cycles in half cells and 94.5% retention after 1,000 cycles in full cells. This redefined single-crystal cathode represents a significant step towards the industrial adoption of high-energy-density materials.

Date: 2025
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DOI: 10.1038/s41560-025-01827-4

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