The roles of subsurface carbon and hydrogen in palladium-catalyzed alkyne hydrogenation

Teschner, D., Borsodi, J., Wootsch, A., Revay, Z., Havecker, M., Knop-Gericke, A., Jackson, S.D. and Schlogl, R. (2008) The roles of subsurface carbon and hydrogen in palladium-catalyzed alkyne hydrogenation. Science, 320(5872), pp. 86-89. (doi:10.1126/science.1155200)

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Abstract

Alkynes can be selectively hydrogenated into alkenes on solid palladium catalysts. This process requires a strong modification of the near- surface region of palladium, in which carbon ( from fragmented feed molecules) occupies interstitial lattice sites. In situ x- ray photoelectron spectroscopic measurements under reaction conditions indicated that much less carbon was dissolved in palladium during unselective, total hydrogenation. Additional studies of hydrogen content using in situ prompt gamma activation analysis, which allowed us to follow the hydrogen content of palladium during catalysis, indicated that unselective hydrogenation proceeds on hydrogen- saturated beta- hydride, whereas selective hydrogenation was only possible after decoupling bulk properties from the surface events. Thus, the population of subsurface sites of palladium, by either hydrogen or carbon, governs the hydrogenation events on the surface.

Item Type:Articles
Keywords:ACTIVATION ALKENES ALKYNE HYDROGENATION CARBON CATALYSIS CATALYST CATALYSTS ETHENE heterogeneous catalysis HYDROGEN HYDROGENATION IMPURITIES IN-SITU LATTICE METHANOL OXIDATION MOLECULE MOLECULES NANOPARTICLES Palladium PALLADIUM CATALYSTS SURFACE
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Jackson, Professor Samuel
Authors: Teschner, D., Borsodi, J., Wootsch, A., Revay, Z., Havecker, M., Knop-Gericke, A., Jackson, S.D., and Schlogl, R.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Science
Publisher:American Association for the Advancement of Science
ISSN:0036-8075
ISSN (Online):1095-9203

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
298521Advanced Technology in Catalytic Chemistry and Engineering for Novel Applications (ATHENA)Samuel JacksonEngineering & Physical Sciences Research Council (EPSRC)GR/R50899/01Chemistry