Selective liquid-phase oxidation of alcohols catalyzed by a silver-based catalyst promoted by the presence of ceria

被引:124
作者
Beier, Matthias J. [1 ]
Hansen, Thomas W. [2 ]
Grunwaldt, Jan-Dierk [1 ]
机构
[1] Tech Univ Denmark, Dept Chem & Biochem Engn, DK-2800 Lyngby, Denmark
[2] Tech Univ Denmark, Ctr Elect Nanoscopy, DK-2800 Lyngby, Denmark
关键词
Selective alcohol oxidation; Silver catalysis; Molecular oxygen; X-ray absorption spectroscopy; Cold catalysts; Catalyst screening; Ceria; SUPERCRITICAL CARBON-DIOXIDE; SUPPORTED GOLD NANOPARTICLES; RAY-ABSORPTION SPECTROSCOPY; BENZYL ALCOHOL; AEROBIC OXIDATION; MOLECULAR-OXYGEN; METAL-CATALYSTS; HETEROGENEOUS CATALYSIS; REACTION-MECHANISM; FINE-STRUCTURE;
D O I
10.1016/j.jcat.2009.06.022
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A number of silver catalysts Supported on SiO2, Al2O3, Celite, CeO2, kaolin, MgO, and activated carbon were screened for their catalytic activity in the selective liquid-phase oxidation of benzyl alcohol using a special screening approach. For this purpose 5-6 catalyst samples were mixed and tested simultaneously. When a high catalytic conversion (>30% over 2 h) was found the number of catalyst components was reduced in the following tests. Thereby, a collaborative effect between a physical mixture of ceria nanoparticles and silver-impregnated silica (10 wt.% Ag-SiO2) was found. The catalytic activity was highly dependent on the silver loading, the amount of ceria, and especially the calcination procedure. Transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray absorption spectroscopy (XANES, EXAFS) demonstrate that silver is mainly present as metallic particles. This is also supported by in situ XAS experiments. Oxygen species incorporated in the silver lattice appear to be important for the catalytic oxidation of the alcohol for which a preliminary mechanism is presented. The application of the catalyst was extended to the oxidation of a wide range of primary and secondary alcohols. Compared to palladium and gold catalysts, the new silver catalyst performed similarly or even superior in the presence of CeO2. In addition, the presence of ceria increased the catalytic activity of all investigated catalysts. (C) 2009 Elsevier Inc. All rights reserved.
引用
收藏
页码:320 / 330
页数:11
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