Journal article

In situ observation of oscillatory redox dynamics of copper.

  • Cao J Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Rinaldi A Chemistry Department, King Fahd University of Petroleum & Minerals, 31261, Dhahran, Saudi Arabia.
  • Plodinec M Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Huang X Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Willinger E Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Hammud A Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Hieke S Max-Planck-Institut für Eisenforschung GmbH, 40237, Düsseldorf, Germany.
  • Beeg S Max Planck Institute for Chemical Energy Conversion, 45470, Mülheim an der Ruhr, Germany.
  • Gregoratti L Elettra-Sincrotrone Trieste S.C.p.A, 34149, Basovizza, Trieste, Italy.
  • Colbea C Scientific Center for Optical and Electron Microscopy, ScopeMETH Zürich, 8093, Zürich, Switzerland.
  • Schlögl R Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany.
  • Antonietti M Max-Planck-Institute of Colloids and Interfaces, Department of Colloid Chemistry, 14424, Potsdam, Germany.
  • Greiner M Max Planck Institute for Chemical Energy Conversion, 45470, Mülheim an der Ruhr, Germany. mark.greiner@cec.mpg.de.
  • Willinger M Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195, Berlin, Germany. willmarc@ethz.ch.
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  • 2020-07-18
Published in:
  • Nature communications. - 2020
English 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.
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  • English
Open access status
gold
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https://sonar.ch/global/documents/185642
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