期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 17, 期 4, 页码 1247-1256出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201002469
关键词
alcohols; dehydrogenation; gold; heterogeneous catalysis; nanoparticles
资金
- National Natural Science Foundation of China [20625310, 20773099, 20873110, 20923004]
- National Basic Research Program of China [2010CB732303]
- Research Fund for the Doctoral Program of Higher Education [20090121110007]
- Key Scientific Project of Fujian Province [2009HZ0002-1]
Gold nanoparticles with uniform mean sizes (approximate to 3nm) loaded onto various supports have been prepared and studied for the oxidant-free dehydrogenation of benzyl alcohol to benzaldehyde and hydrogen. The use of hydrotalcite (HT), which possesses both strong acidity and strong basicity, provides the best catalytic performance. Au/HT catalysts with various mean Au particle sizes (2.1-21 nm) have been successfully prepared by a deposition precipitation method under controlled conditions. Detailed catalytic reaction studies with these catalysts demonstrate that the Au-catalyzed dehydrogenation of benzyl alcohol is a structure-sensitive reaction. The turnover frequency (TOF) increases with decreasing Au mean particle size (from 12 to 2.1 nm). A steep rise in TOF occurs when the mean Au particle size becomes smaller than 4 nm. Our present work suggests that the acid base properties of the support and the size of Au nanoparticles are two key factors controlling the alcohol dehydrogenation catalysis. A reaction mechanism is proposed to rationalize these results. It is assumed that the activation of the beta C-H bond of alcohol, which requires the coordinatively unsaturated Au atoms, is the rate-determining step.
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