Mohr, Christian ; Hofmeister, Herbert ; Radnik, Jörg ; Claus, Peter (2003)
Identification of active sites in gold-catalyzed hydrogenation of acrolein.
In: Journal Of The American Chemical Society, 125 (7)
doi: 10.1021/ja027321q
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The active sites of supported gold catalysts, favoring the adsorption of CO groups of acrolein and subsequent reaction to allyl alcohol, have been identified as edges of gold nanoparticles. After our recent finding that this reaction preferentially occurs on single crystalline particles rather than multiply twinned ones, this paper reports on a new approach to distinguish different features of the gold particle morphology. Elucidation of the active site issue cannot be simply done by varying the size of gold particles, since the effects of faceting and multiply twinned particles may interfere. Therefore, modification of the gold particle surface by indium has been used to vary the active site characteristics of a suitable catalyst, and a selective decoration of gold particle faces has been observed, leaving edges free. This is in contradiction to theoretical predictions, suggesting a preferred occupation of the low-coordinated edges of the gold particles. On the bimetallic catalyst, the desired allyl alcohol is the main product (selectivity 63%; temperature 593 K, total pressure ptotal = 2 MPa). From the experimentally proven correlation between surface structure and catalytic behavior, the edges of single crystalline gold particles have been identified as active sites for the preferred CO hydrogenation.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2003 |
| Autor(en): | Mohr, Christian ; Hofmeister, Herbert ; Radnik, Jörg ; Claus, Peter |
| Art des Eintrags: | Bibliographie |
| Titel: | Identification of active sites in gold-catalyzed hydrogenation of acrolein |
| Sprache: | Englisch |
| Publikationsjahr: | 2003 |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal Of The American Chemical Society |
| Jahrgang/Volume einer Zeitschrift: | 125 |
| (Heft-)Nummer: | 7 |
| DOI: | 10.1021/ja027321q |
| Kurzbeschreibung (Abstract): | The active sites of supported gold catalysts, favoring the adsorption of CO groups of acrolein and subsequent reaction to allyl alcohol, have been identified as edges of gold nanoparticles. After our recent finding that this reaction preferentially occurs on single crystalline particles rather than multiply twinned ones, this paper reports on a new approach to distinguish different features of the gold particle morphology. Elucidation of the active site issue cannot be simply done by varying the size of gold particles, since the effects of faceting and multiply twinned particles may interfere. Therefore, modification of the gold particle surface by indium has been used to vary the active site characteristics of a suitable catalyst, and a selective decoration of gold particle faces has been observed, leaving edges free. This is in contradiction to theoretical predictions, suggesting a preferred occupation of the low-coordinated edges of the gold particles. On the bimetallic catalyst, the desired allyl alcohol is the main product (selectivity 63%; temperature 593 K, total pressure ptotal = 2 MPa). From the experimentally proven correlation between surface structure and catalytic behavior, the edges of single crystalline gold particles have been identified as active sites for the preferred CO hydrogenation. |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie II 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie |
| Hinterlegungsdatum: | 20 Mär 2009 08:57 |
| Letzte Änderung: | 05 Mär 2013 09:18 |
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