Visualizing catalyst heterogeneity by a multifrequential oscillating reaction

Yuri Suchorski, Martin Datler, Ivan Bespalov, Johannes Zeininger, Michael Stöger-Pollach, Johannes Bernardi, Henrik Grönbeck and Günther Rupprechter ()
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Yuri Suchorski: Technische Universität Wien
Martin Datler: Technische Universität Wien
Ivan Bespalov: Technische Universität Wien
Johannes Zeininger: Technische Universität Wien
Michael Stöger-Pollach: Technische Universität Wien
Johannes Bernardi: Technische Universität Wien
Henrik Grönbeck: Chalmers University of Technology
Günther Rupprechter: Technische Universität Wien

Nature Communications, 2018, vol. 9, issue 1, 1-6

Abstract: Abstract It is well documented that different surface structures of catalytically active metals may exhibit different catalytic properties. This is typically examined by comparing the catalytic activities and/or selectivities of various well-defined smooth and stepped/kinked single crystal surfaces. Here we report the direct observation of the heterogeneity of active polycrystalline surfaces under reaction conditions, which is manifested by multifrequential oscillations during hydrogen oxidation over rhodium, imaged in situ by photoemission electron microscopy. Each specific surface structure, i.e. the crystallographically different µm-sized domains of rhodium, exhibits an individual spiral pattern and oscillation frequency, despite the global diffusional coupling of the surface reaction. This reaction behavior is attributed to the ability of stepped surfaces of high-Miller-index domains to facilitate the formation of subsurface oxygen, serving as feedback mechanism of the observed oscillations. The current experimental findings, backed by microkinetic modeling, may open an alternative approach towards addressing the structure-sensitivity of heterogeneous surfaces.

Date: 2018
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03007-3

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DOI: 10.1038/s41467-018-03007-3

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