Identification of active sites in gold-catalyzed hydrogenation of acrolein.
The active sites of supported gold catalysts, favoring the adsorption of C=O 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 p(total) = 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 C=O hydrogenation.
Mohr
Christian
C
Department of Chemistry, Institute of Chemical Technology II, Darmstadt University of Technology, Petersenstrasse 20, D-64287 Darmstadt, Germany.
Hofmeister
Herbert
H
Radnik
Jörg
J
Claus
Peter
P
D000171:Acrolein / Q000737:chemistry*; D001665:Binding Sites; D002384:Catalysis; D006046:Gold / Q000737:chemistry*; D006865:Hydrogenation; D007204:Indium / Q000737:chemistry; D010084:Oxidation-Reduction; D010316:Particle Size; D020005:Propanols / Q000138:chemical synthesis / Q000737:chemistry; D013499:Surface Properties; D015034:Zinc Oxide / Q000737:chemistry
D020005:Propanols; D007204:Indium; C006463:allyl alcohol; D006046:Gold; D000171:Acrolein; D015034:Zinc Oxide