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Operando real-space imaging of a structural phase transformation in the high-voltage electrode LixNi0.5Mn1.5O4

Author

Listed:
  • Yifei Sun

    (Cornell University)

  • Sunny Hy

    (University of California San Diego)

  • Nelson Hua

    (University of California San Diego
    Paul Scherrer Institute)

  • James Wingert

    (University of California San Diego)

  • Ross Harder

    (Argonne National Laboratory)

  • Ying Shirley Meng

    (University of California San Diego
    University of Chicago)

  • Oleg Shpyrko

    (University of California San Diego)

  • Andrej Singer

    (Cornell University)

Abstract

Discontinuous solid-solid phase transformations play a pivotal role in determining the properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in LixNi0.5Mn1.5O4 within an operational Li metal coin cell. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to a planar semi-coherent interface driven by dislocation dynamics. Our data indicates negligible kinetic limitations from interface propagation impacting the transformation kinetics, even at a discharge rate of C/2 (80 mA/g). This study highlights BCDI’s capability to decode complex operando diffraction data, offering exciting opportunities to study nanoscale phase transformations with various stimuli.

Suggested Citation

  • Yifei Sun & Sunny Hy & Nelson Hua & James Wingert & Ross Harder & Ying Shirley Meng & Oleg Shpyrko & Andrej Singer, 2024. "Operando real-space imaging of a structural phase transformation in the high-voltage electrode LixNi0.5Mn1.5O4," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-55010-6
    DOI: 10.1038/s41467-024-55010-6
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    References listed on IDEAS

    as
    1. Saravanan Kuppan & Yahong Xu & Yijin Liu & Guoying Chen, 2017. "Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy," Nature Communications, Nature, vol. 8(1), pages 1-10, April.
    2. A. Singer & M. Zhang & S. Hy & D. Cela & C. Fang & T. A. Wynn & B. Qiu & Y. Xia & Z. Liu & A. Ulvestad & N. Hua & J. Wingert & H. Liu & M. Sprung & A. V. Zozulya & E. Maxey & R. Harder & Y. S. Meng & , 2018. "Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging," Nature Energy, Nature, vol. 3(8), pages 641-647, August.
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