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Non-topotactic reactions enable high rate capability in Li-rich cathode materials

Author

Listed:
  • Jianping Huang

    (Lawrence Berkeley National Laboratory)

  • Peichen Zhong

    (Lawrence Berkeley National Laboratory
    University of California Berkeley)

  • Yang Ha

    (Lawrence Berkeley National Laboratory)

  • Deok-Hwang Kwon

    (Lawrence Berkeley National Laboratory
    University of California Berkeley)

  • Matthew J. Crafton

    (University of California Berkeley)

  • Yaosen Tian

    (Lawrence Berkeley National Laboratory
    University of California Berkeley)

  • Mahalingam Balasubramanian

    (Argonne National Laboratory)

  • Bryan D. McCloskey

    (University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Wanli Yang

    (Lawrence Berkeley National Laboratory)

  • Gerbrand Ceder

    (Lawrence Berkeley National Laboratory
    University of California Berkeley)

Abstract

High-rate cathode materials for Li-ion batteries require fast Li transport kinetics, which typically rely on topotactic Li intercalation/de-intercalation because it minimally disrupts Li transport pathways. In contrast to this conventional view, here we demonstrate that the rate capability in a Li-rich cation-disordered rocksalt cathode can be significantly improved when the topotactic reaction is replaced by a non-topotactic reaction. The fast non-topotactic lithiation reaction is enabled by facile and reversible transition metal octahedral-to-tetrahedral migration, which improves rather than impedes Li transport. Using this concept, we show that high-rate performance can be achieved in Mn- and Ni-based cation-disordered rocksalt materials when some of the transition metal content can reversibly switch between octahedral and tetrahedral sites. This study provides a new perspective on the design of high-performance cathode materials by demonstrating how the interplay between Li and transition metal migration in materials can be conducive to fast non-topotactic Li intercalation/de-intercalations.

Suggested Citation

  • Jianping Huang & Peichen Zhong & Yang Ha & Deok-Hwang Kwon & Matthew J. Crafton & Yaosen Tian & Mahalingam Balasubramanian & Bryan D. McCloskey & Wanli Yang & Gerbrand Ceder, 2021. "Non-topotactic reactions enable high rate capability in Li-rich cathode materials," Nature Energy, Nature, vol. 6(7), pages 706-714, July.
    • Handle: RePEc:nat:natene:v:6:y:2021:i:7:d:10.1038_s41560-021-00817-6
    DOI: 10.1038/s41560-021-00817-6
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    Cited by:

    1. Xiangkun Kong & Run Gu & Zongzi Jin & Lei Zhang & Chi Zhang & Wenyi Xiang & Cui Li & Kang Zhu & Yifan Xu & Huang Huang & Xiaoye Liu & Ranran Peng & Chengwei Wang, 2024. "Maximizing interface stability in all-solid-state lithium batteries through entropy stabilization and fast kinetics," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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