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Selective oxidation of crotyl alcohol over pd(111)

Lee, Adam Fraser, Chang, Z, Ellis, P, Hackett, S. F. J. and Wilson, Karen 2007. Selective oxidation of crotyl alcohol over pd(111). Journal of Physical Chemistry C 111 (51) , pp. 18844-18847. 10.1021/jp709944c

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The selective oxidation of crotyl alcohol has been explored over a Pd(111) model catalyst. At low temperatures, the alcohol adsorbs intact with the CdC bond parallel to the surface. Activation likely proceeds through an allyl alkoxide intermediate that follows two distinct reaction channels. Over the clean surface, �90% of the alcohol oxidizes to surface bound crotonaldehyde above 200 K, which subsequently all decarbonylates to propene and CO at room temperature. The minor reaction channel involves C-O scission to 2-butene and water. While some of these undesired reactively formed alkene products desorb around 300 K, the majority dehydrogenate to irreversibly bound carbon above 380 K. This latter decomposition pathway is unlikely to be important at the low temperatures utilized in liquid-phase crotyl alcohol oxidation over supported palladium catalysts. Adsorbed CO persists until 430 K and is likely responsible for site-blocking and deactivation of dispersed metallic Pd clusters. Coadsorbed oxygen suppresses crotonaldehyde decarbonylation and promotes its release from the surface.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Subjects: Q Science > QD Chemistry
Publisher: American Chemical Society
ISSN: 19327455
Last Modified: 19 Mar 2016 22:21

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