In situ observation of oscillatory redox dynamics of copper.

Nature Communications
Jing CaoMarc-Georg Willinger

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.

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Citations

Jan 21, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·See Wee CheeBeatriz Roldan Cuenya
Apr 8, 2021·Journal of Physics. Condensed Matter : an Institute of Physics Journal·See Wee CheeBeatriz Roldan Cuenya
Jun 13, 2021·Advanced Materials·Xing HuangMarc-Georg Willinger
Sep 28, 2021·The Journal of Physical Chemistry Letters·Xianhu SunGuangwen Zhou

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Methods Mentioned

BETA
scanning
X-ray
electron diffraction
scanning electron microscopy
transmission electron microscopy

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