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Identification of active sites in gold-catalyzed hydrogenation of acrolein

Mohr, Christian and Hofmeister, Herbert and Radnik, Jörg and Claus, Peter (2003):
Identification of active sites in gold-catalyzed hydrogenation of acrolein.
In: Journal Of The American Chemical Society, pp. 1905-1911, 125, (7), [Online-Edition: http://dx.doi.org/10.1021/ja027321q],
[Article]

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.

Item Type: Article
Erschienen: 2003
Creators: Mohr, Christian and Hofmeister, Herbert and Radnik, Jörg and Claus, Peter
Title: Identification of active sites in gold-catalyzed hydrogenation of acrolein
Language: English
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.

Journal or Publication Title: Journal Of The American Chemical Society
Volume: 125
Number: 7
Divisions: 07 Department of Chemistry
07 Department of Chemistry > Fachgebiet Technische Chemie > Technische Chemie II
07 Department of Chemistry > Fachgebiet Technische Chemie
Date Deposited: 20 Mar 2009 08:57
Official URL: http://dx.doi.org/10.1021/ja027321q
Identification Number: doi:10.1021/ja027321q
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