English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Role of Hydrogen Species in Palladium-Catalyzed Alkyne Hydrogenation

MPS-Authors
/persons/resource/persons22163

Teschner,  Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21396

Borsodi,  Janos
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21743

Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

External Resource
No external resources are shared
Fulltext (public)
There are no public fulltexts stored in PuRe
Supplementary Material (public)
There is no public supplementary material available
Citation

Teschner, D., Borsodi, J., Kis, Z., Szentmiklósi, L., Révay, Z., Knop-Gericke, A., et al. (2010). Role of Hydrogen Species in Palladium-Catalyzed Alkyne Hydrogenation. Journal of Physical Chemistry C, 114(5), 2293-2299. doi:10.1021/jp9103799.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0010-F6B0-C
Abstract
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.