2020-02-26
Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst
Publication
Publication
Nanoscale , Volume 12 - Issue 10 p. 5866- 5875
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.
| Additional Metadata | |
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| RSC | |
| doi.org/10.1039/c9nr10087c | |
| Nanoscale | |
| Organisation | Materials & Surface Science for EUV Lithography |
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Jakub, Z., Hulva, J., Ryan, P., Duncan, D., Payne, D., Bliem, R., … Parkinson, G. (2020). Adsorbate-induced structural evolution changes the mechanism of CO oxidation on a Rh/Fe3O4(001) model catalyst. Nanoscale, 12(10), 5866–5875. doi:10.1039/c9nr10087c |
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