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Issue 10, 2020
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Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst

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Abstract

The structure of a catalyst often changes in reactive environments, and following the structural evolution is crucial for the identification of the catalyst's active phase and reaction mechanism. Here we present an atomic-scale study of CO oxidation on a model Rh/Fe3O4(001) “single-atom” catalyst, which has a very different evolution depending on which of the two reactants, O2 or CO, is adsorbed first. Using temperature-programmed desorption (TPD) combined with scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS), we show that O2 destabilizes Rh atoms, leading to the formation of RhxOy clusters; these catalyze CO oxidation via a Langmuir–Hinshelwood mechanism at temperatures as low as 200 K. If CO adsorbs first, the system is poisoned for direct interaction with O2, and CO oxidation is dominated by a Mars-van-Krevelen pathway at 480 K.

Graphical abstract: Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst

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Supplementary files

Article information


Submitted
27 Nov 2019
Accepted
02 Feb 2020
First published
26 Feb 2020

This article is Open Access

Nanoscale, 2020,12, 5866-5875
Article type
Paper

Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst

Z. Jakub, J. Hulva, P. T. P. Ryan, D. A. Duncan, D. J. Payne, R. Bliem, M. Ulreich, P. Hofegger, F. Kraushofer, M. Meier, M. Schmid, U. Diebold and G. S. Parkinson, Nanoscale, 2020, 12, 5866
DOI: 10.1039/C9NR10087C

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