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Nonpolarizing oxygen-redox capacity without O-O dimerization in Na2Mn3O7

Author

Listed:
  • Akihisa Tsuchimoto

    (The University of Tokyo)

  • Xiang-Mei Shi

    (The University of Tokyo)

  • Kosuke Kawai

    (The University of Tokyo)

  • Benoit Mortemard de Boisse

    (The University of Tokyo)

  • Jun Kikkawa

    (National Institute for Materials Science (NIMS))

  • Daisuke Asakura

    (National Institute of Advanced Industrial Science and Technology (AIST))

  • Masashi Okubo

    (The University of Tokyo
    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University)

  • Atsuo Yamada

    (The University of Tokyo
    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University)

Abstract

Reversibility of an electrode reaction is important for energy-efficient rechargeable batteries with a long battery life. Additional oxygen-redox reactions have become an intensive area of research to achieve a larger specific capacity of the positive electrode materials. However, most oxygen-redox electrodes exhibit a large voltage hysteresis >0.5 V upon charge/discharge, and hence possess unacceptably poor energy efficiency. The hysteresis is thought to originate from the formation of peroxide-like O22− dimers during the oxygen-redox reaction. Therefore, avoiding O-O dimer formation is an essential challenge to overcome. Here, we focus on Na2-xMn3O7, which we recently identified to exhibit a large reversible oxygen-redox capacity with an extremely small polarization of 0.04 V. Using spectroscopic and magnetic measurements, the existence of stable O−• was identified in Na2-xMn3O7. Computations reveal that O−• is thermodynamically favorable over the peroxide-like O22− dimer as a result of hole stabilization through a (σ + π) multiorbital Mn-O bond.

Suggested Citation

  • Akihisa Tsuchimoto & Xiang-Mei Shi & Kosuke Kawai & Benoit Mortemard de Boisse & Jun Kikkawa & Daisuke Asakura & Masashi Okubo & Atsuo Yamada, 2021. "Nonpolarizing oxygen-redox capacity without O-O dimerization in Na2Mn3O7," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-020-20643-w
    DOI: 10.1038/s41467-020-20643-w
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    Cited by:

    1. Xuelong Wang & Liang Yin & Arthur Ronne & Yiman Zhang & Zilin Hu & Sha Tan & Qinchao Wang & Bohang Song & Mengya Li & Xiaohui Rong & Saul Lapidus & Shize Yang & Enyuan Hu & Jue Liu, 2023. "Stabilizing lattice oxygen redox in layered sodium transition metal oxide through spin singlet state," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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