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Bridging the pressure and materials gap: in-depth characterization and reaction studies of silver-catalyzed acrolein hydrogenation

Bron, Michael ; Teschner, Detre ; Knop-Gericke, Axel ; Steinhauer, Bernd ; Scheybal, Andreas ; Hävecker, Michael ; Wang, Di ; Födisch, Ringo ; Hönicke, Dieter ; Wootsch, Attila ; Schlögl, Robert ; Claus, Peter :
Bridging the pressure and materials gap: in-depth characterization and reaction studies of silver-catalyzed acrolein hydrogenation.
[Online-Edition: http://dx.doi.org/10.1016/j.jcat.2005.05.018]
In: Journal of Catalysis, 234 pp. 37-47.
[Artikel], (2005)

Offizielle URL: http://dx.doi.org/10.1016/j.jcat.2005.05.018

Kurzbeschreibung (Abstract)

The gas-phase hydrogenation of acrolein over silver was studied in a broad pressure range from not, vert, similar2 mbar to 20 bar and with various silver materials (single crystals, sputtered silver, silica-supported Ag nanoparticles) in an attempt to examine the question of the “pressure and materials gap” in catalysis. High pressures and nanoparticles favour the formation of allyl alcohol (selectivities up to 42%), whereas with the opposite conditions propionaldehyde is by far the main product. A critical minimum reaction pressure was identified: below ca. 100 mbar, no allyl alcohol was formed. In situ-XAS measurements were performed at 7.5 mbar to gain insight into the interaction of acrolein with silver samples. Despite the fact that beam-induced processes have been observed, it is concluded that at low pressures, acrolein orients parallel to the surface on Ag(111) and is present at the surface in the form of hydrogenated propionaldehyde-like species. The influence of catalyst structure and pressure on the adsorption geometry of acrolein and the possible rate-determining step in acrolein hydrogenation are discussed.

Typ des Eintrags: Artikel
Erschienen: 2005
Autor(en): Bron, Michael ; Teschner, Detre ; Knop-Gericke, Axel ; Steinhauer, Bernd ; Scheybal, Andreas ; Hävecker, Michael ; Wang, Di ; Födisch, Ringo ; Hönicke, Dieter ; Wootsch, Attila ; Schlögl, Robert ; Claus, Peter
Titel: Bridging the pressure and materials gap: in-depth characterization and reaction studies of silver-catalyzed acrolein hydrogenation
Sprache: Englisch
Kurzbeschreibung (Abstract):

The gas-phase hydrogenation of acrolein over silver was studied in a broad pressure range from not, vert, similar2 mbar to 20 bar and with various silver materials (single crystals, sputtered silver, silica-supported Ag nanoparticles) in an attempt to examine the question of the “pressure and materials gap” in catalysis. High pressures and nanoparticles favour the formation of allyl alcohol (selectivities up to 42%), whereas with the opposite conditions propionaldehyde is by far the main product. A critical minimum reaction pressure was identified: below ca. 100 mbar, no allyl alcohol was formed. In situ-XAS measurements were performed at 7.5 mbar to gain insight into the interaction of acrolein with silver samples. Despite the fact that beam-induced processes have been observed, it is concluded that at low pressures, acrolein orients parallel to the surface on Ag(111) and is present at the surface in the form of hydrogenated propionaldehyde-like species. The influence of catalyst structure and pressure on the adsorption geometry of acrolein and the possible rate-determining step in acrolein hydrogenation are discussed.

Titel der Zeitschrift, Zeitung oder Schriftenreihe: Journal of Catalysis
Band: 234
Verlag: Elsevier Inc.
Freie Schlagworte: Acrolein; Silver; Selective Hydrogenation; Pressure gap; Materials gap; In situ-XAS
Fachbereich(e)/-gebiet(e): Fachbereich Chemie
Fachbereich Chemie > Technische Chemie > Technische Chemie II
Fachbereich Chemie > Technische Chemie
Hinterlegungsdatum: 20 Mär 2009 08:48
Offizielle URL: http://dx.doi.org/10.1016/j.jcat.2005.05.018
ID-Nummer: 10.1016/j.jcat.2005.05.018
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