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RESEARCH PRODUCT

CO Oxidation on Cationic Gold Clusters: A Theoretical Study

Antonio PrestianniFrédéric LabatCarlo AdamoAntonino MartoranaIlaria Ciofini

subject

Latter mechanismInorganic chemistryReaction pathPhotochemistryChemical reactionNeutral clusterNanoclustersCatalysisMolecular specieAdsorptionCompetitive interactionCluster (physics)Reactivity (chemistry)Physical and Theoretical ChemistrySupported golds Engineering main heading: Carbon monoxideEngineering controlled terms: AdsorptionPositively chargedOxidation Engineering uncontrolled terms: Catalytic siteDioxygenChemistryElementary stepCationic polymerizationOxidation of COCatalytic oxidationCO oxidationSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsFlow interactionGeneral EnergyCarbon dioxideCatalytic oxidationChemical oxygen demandCarbon clusterCationic gold clusterChemical reactionGold compound

description

Aiming at understanding the elementary steps governing the oxidation of CO catalyzed by dispersed or supported gold nanoclusters, the reactivity of molecular species, such as O2 and CO, on neutral and positively charged Au13 clusters have been studied using a DFT approach. Two CO oxidation mechanisms have been simulated, involving respectively the adsorption of CO and O2 on adjacent catalytic sites (two-sites mechanism) and the competitive interaction of the reactants on the same site (single-site mechanism). It is demonstrated that in the former scheme a definite interaction of CO and O2 with both the charged and neutral cluster is effective, but that a chemical reaction between the adsorbates does not take place. Only the latter mechanism on positively charged Au13 cluster can give rise to the rupture of dioxygen and carbon dioxide formation. Detailed reaction paths corresponding to this case are calculated.

yearjournalcountryeditionlanguage
2008-10-24The Journal of Physical Chemistry C
https://doi.org/10.1021/jp8062959