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          Institute: Fritz-Haber-Institut     Collection: Inorganic Chemistry     Display Documents

ID: 462677.0, Fritz-Haber-Institut / Inorganic Chemistry
Role of Hydrogen Species in Palladium-Catalyzed Alkyne Hydrogenation
Authors:Teschner, Detre; Borsodi, János; Kis, Zoltán; Szentmiklósi, László; Révay, Zsolt; Knop-Gericke, Axel; Schlögl, Robert; Torres, Daniel; Sautet, Philippe
Research Context:Pd catalysts
Date of Publication (YYYY-MM-DD):2010-01
Title of Journal:Journal of Physical Chemistry C
Journal Abbrev.:J. Phys. Chem. C
Issue / Number:5
Start Page:2293
End Page:2299
Copyright:© 2010 American Chemical Society
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:Selective alkyne hydrogenation in the presence of carbon-carbon double bond compounds, for which Pd is an excellent catalyst, is a strategically important large-scale industrial process. Although in palladium, functionality and structure are closely interrelated, knowledge of the structure of Pd is insufficient as the interaction with the chemical environment causes drastic compositional changes near the subsurface region: while unselective hydrogenation proceeds in the presence of a β-hydride phase, selective hydrogenation can be achieved only in the presence of a near-surface Pd-C phase. Here, we show from a combination of in situ prompt gamma activation analysis and ab initio simulations based on density functional theory that (i) the presence of the Pd-C phase created under selective conditions implies a strong change in the surface and subsurface stability of hydrogen, (ii) there is still a slower exchange of bulk and surface hydrogen, and (iii) the reaction rate for selective hydrogenation is independent of the bulk H/Pd ratio.
Free Keywords:Palladium; hydrogen; in situ PGAA; DFT; isotope exchange
External Publication Status:published
Document Type:Article
Communicated by:Robert Schlögl
Affiliations:Fritz-Haber-Institut/Inorganic Chemistry/Electronic Structure and Adsorption / Metals
Fritz-Haber-Institut/Inorganic Chemistry/Inorganic Chemistry
External Affiliations:Institute of Isotopes, Hungarian Academy of Science, POB 77, Budapest, H-1525, Hungary,
Université de Lyon, CNRS, Institut de Chimie, Laboratoire de Chimie, Ecole Normale Suprieure de Lyon, 46 Allée d’Italie, 69364 Lyon, Cedex 07, France
Identifiers:URL:http://dx.doi.org/10.1021/jp9103799 [only for subscriber]
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