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Delocalized electron holes on oxygen in a battery cathode

Author

Listed:
  • Robert A. House

    (University of Oxford)

  • Gregory J. Rees

    (University of Oxford)

  • Kit McColl

    (University of Bath)

  • John-Joseph Marie

    (University of Oxford)

  • Mirian Garcia-Fernandez

    (Diamond Light Source)

  • Abhishek Nag

    (Diamond Light Source)

  • Ke-Jin Zhou

    (Diamond Light Source)

  • Simon Cassidy

    (University of Oxford)

  • Benjamin J. Morgan

    (University of Bath)

  • M. Saiful Islam

    (University of Oxford)

  • Peter G. Bruce

    (University of Oxford
    University of Oxford)

Abstract

Oxide ions in transition metal oxide cathodes can store charge at high voltage offering a route towards higher energy density batteries. However, upon charging these cathodes, the oxidized oxide ions condense to form molecular O2 trapped in the material. Consequently, the discharge voltage is much lower than charge, leading to undesirable voltage hysteresis. Here we capture the nature of the electron holes on O2− before O2 formation by exploiting the suppressed transition metal rearrangement in ribbon-ordered Na0.6[Li0.2Mn0.8]O2. We show that the electron holes formed are delocalized across the oxide ions coordinated to two Mn (O–Mn2) arranged in ribbons in the transition metal layers. Furthermore, we track these delocalized hole states as they gradually localize in the structure in the form of trapped molecular O2 over a period of days. Establishing the nature of hole states on oxide ions is important if truly reversible high-voltage O-redox cathodes are to be realized.

Suggested Citation

  • Robert A. House & Gregory J. Rees & Kit McColl & John-Joseph Marie & Mirian Garcia-Fernandez & Abhishek Nag & Ke-Jin Zhou & Simon Cassidy & Benjamin J. Morgan & M. Saiful Islam & Peter G. Bruce, 2023. "Delocalized electron holes on oxygen in a battery cathode," Nature Energy, Nature, vol. 8(4), pages 351-360, April.
  • Handle: RePEc:nat:natene:v:8:y:2023:i:4:d:10.1038_s41560-023-01211-0
    DOI: 10.1038/s41560-023-01211-0
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    Cited by:

    1. Tianwei Cui & Jialiang Xu & Xin Wang & Longxiang Liu & Yuxuan Xiang & Hong Zhu & Xiang Li & Yongzhu Fu, 2024. "Highly reversible transition metal migration in superstructure-free Li-rich oxide boosting voltage stability and redox symmetry," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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