CO oxidation on cationic gold clusters: A theoretical study

Antonio Prestianni; Antonino Martorana; Frédéric Labat; Ilaria Ciofini; Carlo Adamo

CO oxidation on cationic gold clusters: A theoretical study

Antonio Prestianni, Antonino Martorana, Frédéric Labat, Ilaria Ciofini, Carlo Adamo

Fisica e Chimica - Emilio Segrè

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Abstract

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.

Original language	English
Number of pages	6
Journal	JOURNAL OF PHYSICAL CHEMISTRY. C
Volume	112
Publication status	Published - 2008

All Science Journal Classification (ASJC) codes

Electronic, Optical and Magnetic Materials
Energy(all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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title = "CO oxidation on cationic gold clusters: A theoretical study",

abstract = "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.",

keywords = "CO oxidations, Carbon clusters, Carbon dioxide, Catalytic oxidation, Cationic gold clusters, Chemical oxygen demand, Chemical reactions, Competitive interactions, Dioxygen, Elementary steps, Engineering controlled terms: Adsorption, Flow interactions, Gold compounds, Latter mechanisms, Molecular species, Neutral clusters, Oxidation Engineering uncontrolled terms: Catalytic sites, Oxidation of CO, Positively charged, Reaction paths, Supported golds Engineering main heading: Carbon monoxide, CO oxidations, Carbon clusters, Carbon dioxide, Catalytic oxidation, Cationic gold clusters, Chemical oxygen demand, Chemical reactions, Competitive interactions, Dioxygen, Elementary steps, Engineering controlled terms: Adsorption, Flow interactions, Gold compounds, Latter mechanisms, Molecular species, Neutral clusters, Oxidation Engineering uncontrolled terms: Catalytic sites, Oxidation of CO, Positively charged, Reaction paths, Supported golds Engineering main heading: Carbon monoxide",

author = "Antonio Prestianni and Antonino Martorana and Fr{\'e}d{\'e}ric Labat and Ilaria Ciofini and Carlo Adamo",

year = "2008",

language = "English",

volume = "112",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

publisher = "American Chemical Society",

}

TY - JOUR

T1 - CO oxidation on cationic gold clusters: A theoretical study

AU - Prestianni, Antonio

AU - Martorana, Antonino

AU - Labat, Frédéric

AU - Ciofini, Ilaria

AU - Adamo, Carlo

PY - 2008

Y1 - 2008

N2 - 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.

AB - 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.

KW - CO oxidations

KW - Carbon clusters

KW - Carbon dioxide

KW - Catalytic oxidation

KW - Cationic gold clusters

KW - Chemical oxygen demand

KW - Chemical reactions

KW - Competitive interactions

KW - Dioxygen

KW - Elementary steps

KW - Engineering controlled terms: Adsorption

KW - Flow interactions

KW - Gold compounds

KW - Latter mechanisms

KW - Molecular species

KW - Neutral clusters

KW - Oxidation Engineering uncontrolled terms: Catalytic sites

KW - Oxidation of CO

KW - Positively charged

KW - Reaction paths

KW - Supported golds Engineering main heading: Carbon monoxide