Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 47, Pages 13999-14002Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201507368
Keywords
Mars-van Krevelen mechanism; metal-support interactions; oxide surfaces; scanning probe microscopy; supported catalysts
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Funding
- Centre for Atomic-Level Catalyst Design, an Energy Frontier Research Centre - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001058]
- Austrian Science Fund [P24925-N20]
- Vienna University of Technology
- Austrian Science Fund as part of the doctoral college SOLIDS4FUN [W1243]
- European Research Council (Advanced Grant OxideSurfaces)
- European Regional Development Fund (CEITEC) [CZ.1.05/1.1.00/02.0068]
- Austrian Science Fund (FWF) [P 24925] Funding Source: researchfish
- Austrian Science Fund (FWF) [W1243, P24925] Funding Source: Austrian Science Fund (FWF)
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Metal-support interactions are frequently invoked to explain the enhanced catalytic activity of metal nanoparticles dispersed over reducible metal oxide supports, yet the atomic-scale mechanisms are rarely known. In this report, scanning tunneling microscopy was used to study a Pt1-6/Fe3O4 model catalyst exposed to CO, H-2, O-2, and mixtures thereof at 550 K. CO extracts lattice oxygen atoms at the cluster perimeter to form CO2, creating large holes in the metal oxide surface. H-2 and O-2 dissociate on the metal clusters and spill over onto the support. The former creates surface hydroxy groups, which react with the support, ultimately leading to the desorption of water, while oxygen atoms react with Fe from the bulk to create new Fe3O4(001) islands. The presence of the Pt is crucial because it catalyzes reactions that already occur on the bare iron oxide surface, but only at higher temperatures.
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