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

Author

Listed:
  • 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)

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.

Suggested Citation

  • Qimeng Zhang & Jing Wang & Youqi Chu & Weiyuan Huang & Xiaojing Huang & Xianghui Xiao & Lu Ma & Tongchao Liu & Khalil Amine & Jun Lu & Chenghao Yang, 2025. "Intralattice-bonded phase-engineered ultrahigh-Ni single-crystalline cathodes suppress strain evolution," Nature Energy, Nature, vol. 10(8), pages 1001-1012, August.
    • Handle: RePEc:nat:natene:v:10:y:2025:i:8:d:10.1038_s41560-025-01827-4
    DOI: 10.1038/s41560-025-01827-4
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