Selective Amplification of C=O Bond Hydrogenation on Pt/TiO2: Catalytic Reaction and Sum- Frequency Generation Vibrational Spectroscopy Studies of Crotonaldehyde Hydrogenation

被引：120

作者：

Kennedy, Griffin ^{[1
,2
,3
]}

Baker, L. Robert ^{[1
,2
,3
]}

Somorjai, Gabor A. ^{[1
,2
,3
]}

机构：

[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[2] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA

[3] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2014年 / 53卷 / 13期

关键词：

alcohols; heterogeneous catalysis; hydrogenation; platinum; vibrational spectroscopy; METAL-SUPPORT INTERACTIONS; SINGLE-CRYSTAL SURFACES; ALPHA; BETA-UNSATURATED ALDEHYDES; CARBON-MONOXIDE; TITANIUM-OXIDE; LEWIS ACIDITY; PROMOTION; PLATINUM; PT(111); PT/TIO2;

D O I：

10.1002/anie.201400081

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The hydrogenation of crotonaldehyde in the presence of supported platinum nanoparticles was used to determine how the interaction between the metal particles and their support can control catalytic performance. Using gas-phase catalytic reaction studies and insitu sum-frequency generation vibrational spectroscopy (SFG) to study Pt/TiO2 and Pt/SiO2 catalysts, a unique reaction pathway was identified for Pt/TiO2, which selectively produces alcohol products. The catalytic and spectroscopic data obtained for the Pt/SiO2 catalyst shows that SiO2 has no active role in this reaction. SFG spectra obtained for the Pt/TiO2 catalyst indicate the presence of a crotyl-oxy surface intermediate. By adsorption through the aldehyde oxygen atom to an O-vacancy site on the TiO2 surface, the CO bond of crotonaldehyde is activated, by charge transfer, for hydrogenation. This intermediate reacts with spillover H provided by the Pt to produce crotyl alcohol.

引用

页码：3405 / 3408

页数：4

共 27 条

[1] Pt/CeO2 catalysts in crotonaldehyde hydrogenation:: Selectivity, metal particle size and SMSI states [J].