H/D exchange reaction on mono-disperse Pt clusters: enhanced activity from minute O concentrations

The H 2 /D 2 exchange reaction was studied on mono-disperse Pt 8 clusters in a μ-reactor. The chemical activity was studied at temperatures varying from room temperature to 180 °C using mass spectrometry. It was found that minute amounts of O 2 in the gas stream increased the chemical activity signi...

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Veröffentlicht in:Catalysis science & technology 2016-09, Vol.6 (18), p.6893-69
Hauptverfasser: Riedel, Jakob Nordheim, Rötzer, Marian David, Jørgensen, Mikkel, Vej-Hansen, Ulrik Grønbjerg, Pedersen, Thomas, Sebok, Bela, Schweinberger, Florian Frank, Vesborg, Peter Christian Kjærgaard, Hansen, Ole, Schiøtz, Jakob, Heiz, Ulrich, Chorkendorff, Ib
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Zusammenfassung:The H 2 /D 2 exchange reaction was studied on mono-disperse Pt 8 clusters in a μ-reactor. The chemical activity was studied at temperatures varying from room temperature to 180 °C using mass spectrometry. It was found that minute amounts of O 2 in the gas stream increased the chemical activity significantly. XPS and ISS before and after reaction suggest little or no sintering during reaction. A reaction pathway is suggested based on DFT. H 2 desorption is identified as the rate-limiting step and O 2 is confirmed as the source of the increased activity. The binding energy of platinum atoms in a SiO 2 supported Pt 8 cluster is found to be comparable to the interatomic binding energies of bulk platinum, underlining the stability of the model system. Hydrogen dissociation on mono-disperse platinum clusters is found to increase with minute amounts of oxygen in the gas stream.
ISSN:2044-4753
2044-4761
DOI:10.1039/c6cy00756b