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Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution

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    Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution
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    † †Physical & Computational Sciences Directorate,§Institute for Integrated Catalysis and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
    ‡ Department of Chemistry and Catalysis Research Center, Technische Universität München, Garching 85748, Germany
    National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
    # Department of Materials Science and Engineering, University of Washington, Seattle, Washington 98195, United States
    *[email protected]
    *[email protected]
    *[email protected]
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    Cite this: J. Am. Chem. Soc. 2017, 139, 36, 12342–12345
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    https://doi.org/10.1021/jacs.7b05240
    Published August 21, 2017
    Copyright © 2017 American Chemical Society
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    Abstract

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    A novel pathway of increasing the surface density of catalytically active oxygen radical sites on a MoVTeNb oxide (M1 phase) catalyst during alkane oxidative dehydrogenation is reported. The novel sites form when a fraction of Te4+ is reduced and emitted from the M1 crystals under catalytic operating conditions, without compromising structural integrity of the catalyst framework. Density functional theory calculations show this Te reduction induces multiple inter-related electron transfers, and the associated cooperative effects lead to the formation of O– radicals. The in situ observations identify complex dynamic changes in the catalyst on an atomistic level, highlighting a new way to tailor structure and dynamics for highly active catalysts.

    Copyright © 2017 American Chemical Society

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    • Catalyst synthesis, ESTEM experiment details, additional DFT information and catalyst kinetic test (PDF)

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    Cite this: J. Am. Chem. Soc. 2017, 139, 36, 12342–12345
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.7b05240
    Published August 21, 2017
    Copyright © 2017 American Chemical Society
    Request reuse permissions

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