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Oxygen Redox Activity through a Reductive Coupling Mechanism in the P3-Type Nickel-Doped Sodium Manganese Oxide

  • Eun Jeong Kim
    Eun Jeong Kim
    School of Chemistry, University of St. Andrews, St. Andrews, Fife, KY16 9ST, United Kingdom
    ALISTORE-ERI, 80039, Amiens Cedex, France
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  • , 
  • Le Anh Ma
    Le Anh Ma
    Ångström Advanced Battery Centre, Department of Chemistry Ångström Laboratory, Uppsala University, Uppsala, SE-75121, Sweden
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  • , 
  • Laurent C. Duda
    Laurent C. Duda
    Department of Physics and Astronomy, Division of Molecular and Condensed Matter Physics, Uppsala University, Uppsala, S-75120, Sweden
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    Orcidhttp://orcid.org/0000-0001-8471-0955
  • , 
  • David M. Pickup
    David M. Pickup
    School of Physical Sciences, University of Kent, Canterbury, Kent CT2 7NH, United Kingdom
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  • , 
  • Alan V. Chadwick
    Alan V. Chadwick
    School of Physical Sciences, University of Kent, Canterbury, Kent CT2 7NH, United Kingdom
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    Orcidhttp://orcid.org/0000-0002-6485-9207
  • , 
  • Reza Younesi
    Reza Younesi
    ALISTORE-ERI, 80039, Amiens Cedex, France
    Ångström Advanced Battery Centre, Department of Chemistry Ångström Laboratory, Uppsala University, Uppsala, SE-75121, Sweden
    More by Reza Younesi
    Orcidhttp://orcid.org/0000-0003-2538-8104
  • , 
  • John T. S. Irvine
    John T. S. Irvine
    School of Chemistry, University of St. Andrews, St. Andrews, Fife, KY16 9ST, United Kingdom
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    Orcidhttp://orcid.org/0000-0002-8394-3359
  • , and 
  • A. Robert Armstrong*
    A. Robert Armstrong
    School of Chemistry, University of St. Andrews, St. Andrews, Fife, KY16 9ST, United Kingdom
    ALISTORE-ERI, 80039, Amiens Cedex, France
    *E-mail: [email protected]
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    Orcidhttp://orcid.org/0000-0003-1937-0936
Cite this: ACS Appl. Energy Mater. 2020, 3, 1, 184–191
Publication Date (Web):December 26, 2019
https://doi.org/10.1021/acsaem.9b02171
Copyright © 2019 American Chemical Society
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    Abstract

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    Increasing dependence on rechargeable batteries for energy storage calls for the improvement of energy density of batteries. Toward this goal, introduction of positive electrode materials with high voltage and/or high capacity is in high demand. The use of oxygen chemistry in lithium and sodium layered oxides has been of interest to achieve high capacity. Nevertheless, a complete understanding of oxygen-based redox processes remains elusive especially in sodium ion batteries. Herein, a novel P3-type Na0.67Ni0.2Mn0.8O2, synthesized at low temperature, exhibits oxygen redox activity in high potentials. Characterization using a range of spectroscopic techniques reveals the anionic redox activity is stabilized by the reduction of Ni, because of the strong Ni 3d–O 2p hybridization states created during charge. This observation suggests that different route of oxygen redox processes occur in P3 structure materials, which can lead to the exploration of oxygen redox chemistry for further development in rechargeable batteries.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.9b02171.

    • Rietveld refinement results; ex situ PND patterns; CV; variation of Mn oxidation states; O K-edge SXAS in TEY mode; O K-edge RIXS spectra (PDF)

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