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Ultrastable cathodes enabled by compositional and structural dual-gradient design

Author

Listed:
  • Tongchao Liu

    (Argonne National Laboratory)

  • Lei Yu

    (Argonne National Laboratory)

  • Junxiang Liu

    (Argonne National Laboratory)

  • Alvin Dai

    (Argonne National Laboratory)

  • Tao Zhou

    (Argonne National Laboratory)

  • Jing Wang

    (Argonne National Laboratory)

  • Weiyuan Huang

    (Argonne National Laboratory)

  • Luxi Li

    (Argonne National Laboratory)

  • Matthew Li

    (Argonne National Laboratory)

  • Tianyi Li

    (Argonne National Laboratory)

  • Xiaojing Huang

    (Brookhaven National Laboratory)

  • Xianghui Xiao

    (Brookhaven National Laboratory)

  • Mingyuan Ge

    (Brookhaven National Laboratory)

  • Lu Ma

    (Brookhaven National Laboratory)

  • Zengqing Zhuo

    (Lawrence Berkeley National Laboratory)

  • Rachid Amine

    (Argonne National Laboratory)

  • Yong S. Chu

    (Brookhaven National Laboratory)

  • Wah-Keat Lee

    (Brookhaven National Laboratory)

  • Jianguo Wen

    (Argonne National Laboratory)

  • Khalil Amine

    (Argonne National Laboratory)

Abstract

Cathodes for next-generation batteries are pressed for higher voltage operation (≥4.5 V) to achieve high capacity with long cyclability and thermal tolerance. Current cathodes fail to meet these requirements owing to structural and electrochemical strains at high voltages, leading to fast capacity fading. Here we present a cathode with a coherent architecture ranging from ordered to disordered frameworks with concentration gradient and controllable Ni oxidation activities, which can overcome voltage ceilings imposed by existing cathodes. This design enables simultaneous high-capacity and high-voltage operation at 4.5 V without capacity fading, and up to 4.7 V with negligible capacity decay. Multiscale diffraction and imaging techniques reveal the disordered surface is electrochemically and structurally indestructible, preventing surface parasitic reactions and phase transitions. Structural coherence from ordering to disordering limits lattice parameter changes, mitigating lattice strain and enhancing morphological integrity. The dual-gradient design also notably improves thermal stability, driving the advancement of high-performance cathode materials.

Suggested Citation

  • Tongchao Liu & Lei Yu & Junxiang Liu & Alvin Dai & Tao Zhou & Jing Wang & Weiyuan Huang & Luxi Li & Matthew Li & Tianyi Li & Xiaojing Huang & Xianghui Xiao & Mingyuan Ge & Lu Ma & Zengqing Zhuo & Rach, 2024. "Ultrastable cathodes enabled by compositional and structural dual-gradient design," Nature Energy, Nature, vol. 9(10), pages 1252-1263, October.
  • Handle: RePEc:nat:natene:v:9:y:2024:i:10:d:10.1038_s41560-024-01605-8
    DOI: 10.1038/s41560-024-01605-8
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