Effects of Pd on Catalysis by Au: CO Adsorption, CO Oxidation, and Cyclohexene Hydrogenation by Supported Au and Pd-Au Catalysts - Sorbonne Université Accéder directement au contenu
Article Dans Une Revue ACS Catalysis Année : 2013

Effects of Pd on Catalysis by Au: CO Adsorption, CO Oxidation, and Cyclohexene Hydrogenation by Supported Au and Pd-Au Catalysts

Résumé

catalysts has been shown to have beneficial effects on selective hydrogenation reactions, particularly 1,3- butadiene hydrogenation and the hydrogenation of nitroaromatics, especially p-chloronitrobenzene. Appropriate Pd incorporation enhances hydrogenation activity while maintaining the desirable high selectivity of supported Au catalysts. To better understand this phenomenon, a series of aluminaand titania-supported Au and dilute Pd−Au catalysts were prepared via urea deposition−precipitation. The catalysts were studied with infrared spectroscopy of CO adsorption, CO oxidation catalysis, and cyclohexene hydrogenation catalysis with the goal of understanding how Pd affects the catalytic properties of Au. CO adsorption experiments indicated a substantial amount of surface Pd when the catalyst was under CO. Adsorption experiments at various CO pressures were used to determine CO coverage; application of the Temkin adsorbate interaction model allowed for the determination of adsorption enthalpy metrics for CO adsorption on Au. These experiments showed that Pd induces an electronic effect on Au, affecting both the nascent adsorption enthalpy (ΔH0) and the change in enthalpy with increasing coverage. This electronic modification had little effect on CO oxidation catalysis. Michaelis−Menten kinetics parameters showed essentially the same oxygen reactivity on all the catalysts; the primary differences were in the number of active sites. The bimetallic catalysts were poor cyclohexene hydrogenation catalysts, indicating that there is relatively little exposed Pd when the catalyst is under hydrogen. The results, which are discussed in the context of the literature, indicate that a combination of surface composition and Pd-induced electronic effects on Au appear to increase hydrogen chemisorption and hydrogenation activity while largely maintaining the selectivities associated with catalysis by Au.

Dates et versions

hal-00913284 , version 1 (03-12-2013)

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Citer

Anthony Ward, Laurent Delannoy, Ruth Hahn, Shane Kendell, Christopher J. Pursell, et al.. Effects of Pd on Catalysis by Au: CO Adsorption, CO Oxidation, and Cyclohexene Hydrogenation by Supported Au and Pd-Au Catalysts. ACS Catalysis, 2013, 3, pp.2644-2653. ⟨10.1021/cs400569v⟩. ⟨hal-00913284⟩
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