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<p>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 LiNi<sub>0.92</sub>Co<sub>0.03</sub>Mn<sub>0.05</sub>O<sub>2</sub> (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.</p>

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

  • 期刊论文

  • 发表日期：

    2025年8月12日

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  • Qimeng Zhang,
  • Jing Wang,
  • Youqi Chu,
  • Weiyuan Huang,
  • Xiaojing Huang,
  • Xianghui Xiao,
  • Lu Ma,
  • Tongchao Liu,
  • Khalil Amine,
  • Jun Lu,
  • Chenghao Yang

摘要

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.