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O: Fachverband Oberflächenphysik
O 119: Oxides III: Single-Atom Catalysis, Iron Oxides
O 119.3: Vortrag
Freitag, 20. März 2020, 11:15–11:30, REC C 213
Atomic-Scale Studies of Hydroformylation on Rh1/Fe3O4(001) — •Manuel Ulreich1, Zdeněk Jakub1, Florian Kraushofer1, Matthias Meier1,2, Michael Schmid1, Ulrike Diebold1, Cesare Franchini2, and Gareth S. Parkinson1 — 1Institute of Applied Physics, TU Wien, 1040 Vienna, Austria — 2Center for Computational Materials Science, University of Vienna, 1090 Vienna, Austria
Hydroformylation (alkene + CO + H2 → aldehyde) is an important industrial reaction typically performed in solution using highly-selective mononuclear complexes. Recently, Rh-based “single-atom” catalysts (SACs) have been shown to catalyze this reaction heterogeneously with similar levels of selectivity, suggesting SAC can be a strategy to heterogenize problematic reactions. The main advantage of heterogeneous catalysis is easy separation of the catalyst from the products. SAC is intended to unify this advantage with the high selectivity and activity of homogeneous catalysis. In this talk, TPD and XPS are used to study the coadsorption of ethylene and carbon monoxide on isolated Rh1 adatoms on Fe3O4(001), a critical first step in the hydroformylation reaction. Our results show that 2-fold coordinated Rh1 adatoms on Fe3O4(001) are able to coadsorb C2H4 and CO, but 5-fold coordinated Rh1 adatoms cannot. We conclude that gaining control of the active site geometry is key to the development of highly-selective single-atom catalysis.