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In situ observation of oscillatory redox dynamics of copper

Author

Listed:
  • Jing Cao

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Ali Rinaldi

    (King Fahd University of Petroleum & Minerals)

  • Milivoj Plodinec

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Xing Huang

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft
    ScopeMETH Zürich)

  • Elena Willinger

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft
    ScopeMETH Zürich)

  • Adnan Hammud

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft)

  • Stefan Hieke

    (Max-Planck-Institut für Eisenforschung GmbH)

  • Sebastian Beeg

    (Max Planck Institute for Chemical Energy Conversion)

  • Luca Gregoratti

    (Elettra-Sincrotrone Trieste S.C.p.A)

  • Claudiu Colbea

    (ScopeMETH Zürich)

  • Robert Schlögl

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft
    Max Planck Institute for Chemical Energy Conversion)

  • Markus Antonietti

    (Department of Colloid Chemistry)

  • Mark Greiner

    (Max Planck Institute for Chemical Energy Conversion)

  • Marc Willinger

    (Fritz-Haber-Institut der Max-Planck-Gesellschaft
    ScopeMETH Zürich
    Department of Colloid Chemistry)

Abstract

How a catalyst behaves microscopically under reaction conditions, and what kinds of active sites transiently exist on its surface, is still very much a mystery to the scientific community. Here we present an in situ study on the red-ox behaviour of copper in the model reaction of hydrogen oxidation. Direct imaging combined with on-line mass spectroscopy shows that activity emerges near a phase boundary, where complex spatio-temporal dynamics are induced by the competing action of simultaneously present oxidizing and reducing agents. Using a combination of in situ imaging with in situ X-ray absorption spectroscopy and scanning photoemission microscopy, we reveal the relation between chemical and morphological dynamics and demonstrate that a static picture of active sites is insufficient to describe catalytic function of redox-active metal catalysts. The observed oscillatory redox dynamics provide a unique insight on phase-cooperation and a convenient and general mechanism for constant re-generation of transient active sites.

Suggested Citation

  • Jing Cao & Ali Rinaldi & Milivoj Plodinec & Xing Huang & Elena Willinger & Adnan Hammud & Stefan Hieke & Sebastian Beeg & Luca Gregoratti & Claudiu Colbea & Robert Schlögl & Markus Antonietti & Mark G, 2020. "In situ observation of oscillatory redox dynamics of copper," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17346-7
    DOI: 10.1038/s41467-020-17346-7
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    Cited by:

    1. Shengnan Yue & C. S. Praveen & Alexander Klyushin & Alexey Fedorov & Masahiro Hashimoto & Qian Li & Travis Jones & Panpan Liu & Wenqian Yu & Marc-Georg Willinger & Xing Huang, 2024. "Redox dynamics and surface structures of an active palladium catalyst during methane oxidation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Jan Knudsen & Tamires Gallo & Virgínia Boix & Marie Døvre Strømsheim & Giulio D’Acunto & Christopher Goodwin & Harald Wallander & Suyun Zhu & Markus Soldemo & Patrick Lömker & Filippo Cavalca & Mattia, 2021. "Stroboscopic operando spectroscopy of the dynamics in heterogeneous catalysis by event-averaging," Nature Communications, Nature, vol. 12(1), pages 1-8, December.

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