Durable PROX catalyst based on gold nanoparticles and hydrophobic silica
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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.
CitationDurable PROX catalyst based on gold nanoparticles and hydrophobic silica 2016 Chem. Commun.
PublisherRoyal Society of Chemistry (RSC)
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