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Elucidating the active phases of CoOx films on Au(111) in the CO oxidation reaction

Author

Listed:
  • Hao Chen

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Lorenz J. Falling

    (Lawrence Berkeley National Laboratory
    Lawrence Berkeley National Laboratory)

  • Heath Kersell

    (Lawrence Berkeley National Laboratory
    Biological, and Environmental Engineering, Oregon State University)

  • George Yan

    (University of California, Los Angeles)

  • Xiao Zhao

    (Lawrence Berkeley National Laboratory
    University of California)

  • Judit Oliver-Meseguer

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Max Jaugstetter

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory)

  • Slavomir Nemsak

    (Lawrence Berkeley National Laboratory
    University of California)

  • Adrian Hunt

    (Brookhaven National Laboratory)

  • Iradwikanari Waluyo

    (Brookhaven National Laboratory)

  • Hirohito Ogasawara

    (SLAC National Accelerator Laboratory)

  • Alexis T. Bell

    (Chemical Sciences Division, Lawrence Berkeley National Laboratory
    University of California)

  • Philippe Sautet

    (University of California, Los Angeles
    University of California, Los Angeles)

  • Miquel Salmeron

    (Lawrence Berkeley National Laboratory
    University of California)

Abstract

Noble metals supported on reducible oxides, like CoOx and TiOx, exhibit superior activity in many chemical reactions, but the origin of the increased activity is not well understood. To answer this question we studied thin films of CoOx supported on an Au(111) single crystal surface as a model for the CO oxidation reaction. We show that three reaction regimes exist in response to chemical and topographic restructuring of the CoOx catalyst as a function of reactant gas phase CO/O2 stoichiometry and temperature. Under oxygen-lean conditions and moderate temperatures (≤150 °C), partially oxidized films (CoOx 1) forms containing Co3+ species that are effective in a wide temperature range. Resonant photoemission spectroscopy (ResPES) revealed the unique role of Co3+ sites in catalyzing the CO oxidation. Density function theory (DFT) calculations provided deeper insights into the pathway and free energy barriers for the reactions on these oxide phases. These findings in this work highlight the versatility of catalysts and their evolution to form different active phases, both topological and chemically, in response to reaction conditions exposing a new paradigm in the catalyst structure during operation.

Suggested Citation

  • Hao Chen & Lorenz J. Falling & Heath Kersell & George Yan & Xiao Zhao & Judit Oliver-Meseguer & Max Jaugstetter & Slavomir Nemsak & Adrian Hunt & Iradwikanari Waluyo & Hirohito Ogasawara & Alexis T. B, 2023. "Elucidating the active phases of CoOx films on Au(111) in the CO oxidation reaction," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42301-7
    DOI: 10.1038/s41467-023-42301-7
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    References listed on IDEAS

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    1. Yun Liu & Fan Yang & Yi Zhang & Jianping Xiao & Liang Yu & Qingfei Liu & Yanxiao Ning & Zhiwen Zhou & Hao Chen & Wugen Huang & Ping Liu & Xinhe Bao, 2017. "Enhanced oxidation resistance of active nanostructures via dynamic size effect," Nature Communications, Nature, vol. 8(1), pages 1-7, April.
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