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dc.contributor.authorLaveille, Paco
dc.contributor.authorGuillois, Kevin
dc.contributor.authorTuel, Alain
dc.contributor.authorPetit, Corine
dc.contributor.authorBasset, Jean-Marie
dc.contributor.authorCaps, Valerie
dc.date.accessioned2016-01-24T10:25:34Z
dc.date.available2016-01-24T10:25:34Z
dc.date.issued2016
dc.identifier.citationDurable PROX catalyst based on gold nanoparticles and hydrophobic silica 2016 Chem. Commun.
dc.identifier.issn1359-7345
dc.identifier.issn1364-548X
dc.identifier.pmid26808262
dc.identifier.doi10.1039/C5CC09561A
dc.identifier.urihttp://hdl.handle.net/10754/594734
dc.description.abstract3 nm gold nanoparticles (Au NP) obtained by direct chemical reduction of AuPPh3Cl in the presence of methyl-terminated silica exhibit superior durability for low temperature CO oxidation in the presence of hydrogen (PROX). The activity of hydrophobic Au/SiO2-R972 indeed appears much more stable with time-on-stream than those of the OH-terminated, hydrophilic Au/TiO2 and Au/Al2O3 catalysts, with similar Au NP size. This enhanced stability is attributed to the peculiar catalyst surface of Au/SiO2-R972. Not only may the support hydrophobicity concentrate and facilitate reactant adsorption and product desorption over Au NP, but methyl-terminated SiO2-R972 likely also inhibits carbonatation of the Au/support interface. Hence, at a temperature at which H2/H2O “cleaning” of the carbonate-contaminated Au/Al2O3 and Au/TiO2 surface is inefficient (< 100°C), passivated Au/SiO2-R972 displays much more stable PROX activity. Besides, the virtual absence of surface hydroxyl groups, which provide sites for water formation in H2/O2 atmospheres, can also account for the improved PROX selectivity (>85%) observed over Au/SiO2-R972. This new example, of CO oxidation activity of gold nanoparticles dispersed over a hydrophobic, “inert” support, clearly emphasizes the role of hydrogen as a promoter for the gold-catalyzed oxidation of CO at low temperature. Unlike support-mediated oxygen activation, hydrogen-only mediated oxygen activation takes full advantage of the hydrophobic surface, which is much more resistant against CO2 and thus remains free of poisonous carbonate species, as compared with hydroxyl-terminated catalysts. Hence, although the absence of surface hydroxyl groups prevents the hydrophobic Au/SiO2-R972 catalyst to reach the state-of-the-art activities initially displayed by Au/TiO2 and Au/Al2O3, it brings long-term stability with time-on-stream and superior selectivity, which opens up promising perspectives in the development of viable PROX catalysts based on gold.
dc.language.isoen
dc.publisherRoyal Society of Chemistry (RSC)
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2016/CC/C5CC09561A
dc.rightsArchived with thanks to Chem. Commun.
dc.titleDurable PROX catalyst based on gold nanoparticles and hydrophobic silica
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.identifier.journalChem. Commun.
dc.eprint.versionPost-print
dc.contributor.institutionIRCELYON (Institut de recherches sur la catalyse et l'environnement de Lyon), University of Lyon / CNRS UMR 5256, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex, France
dc.contributor.institutionICPEES (Institut de Chimie et Procédés pour l'Energie, l'Environnement et la Santé), Université de Strasbourg / CNRS UMR 7515, 25 rue Becquerel, 67087 Strasbourg Cedex 2, France
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)
kaust.personLaveille, Paco
kaust.personBasset, Jean-Marie
kaust.personCaps, Valerie
refterms.dateFOA2017-01-20T00:00:00Z


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