Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 18, Issue 11, Pages 7672-7679Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cp00627b
Keywords
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Funding
- European Community [FP7-NMP.2012.1.1-1, 310191]
- Deutsche Forschungsgemeinschaft (DFG)
- Spanish MINECO [CTQ2012-34969, CTQ2015-64618-R]
- Generalitat de Catalunya [2014SGR97, XRQTC]
- Czech Science Foundation [15-06759S]
- COST Action [CM1104]
- ICREA Funding Source: Custom
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The reactivity of atomically dispersed Pt2+ species on the surface of nanostructured CeO2 films and the mechanism of H-2 activation on these sites have been investigated by means of synchrotron radiation photoelectron spectroscopy and resonant photoemission spectroscopy in combination with density functional calculations. Isolated Pt2+ sites are found to be inactive towards H-2 dissociation due to high activation energy required for H-H bond scission. Trace amounts of metallic Pt are necessary to initiate H-2 dissociation on Pt-CeO2 films. H-2 dissociation triggers the reduction of Ce4+ cations which, in turn, is coupled with the reduction of Pt2+ species. The mechanism of Pt2+ reduction involves reverse oxygen spillover and formation of oxygen vacancies on Pt-CeO2 films. Our calculations suggest the existence of a threshold concentration of oxygen vacancies associated with the onset of Pt2+ reduction.
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