Supported gold nanoparticles:: in-depth catalyst characterization and application in hydrogenation and oxidation reactions

被引:294
作者
Schimpf, S
Lucas, M
Mohr, C
Rodemerck, U
Brückner, A
Radnik, J
Hofmeister, H
Claus, P
机构
[1] Tech Univ Darmstadt, Dept Chem, Inst Chem Technol 2, D-64287 Darmstadt, Germany
[2] Dept Catalysis, Inst Appl Chem, Berlin, Germany
[3] Max Planck Inst Microstruct Phys, D-06120 Halle An Der Saale, Germany
关键词
selective hydrogenation; supported gold nanoparticles; carbon monoxide oxidation;
D O I
10.1016/S0920-5861(01)00479-5
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Silica, titania, zirconia and alumina supported gold particles of 1-6 nm size, prepared by various synthetic routes (sol-gel technique, deposition-precipitation, metal organic-chemical vapor deposition, impregnation, dip-coating) were employed in the selective hydrogenation of acrolein, crotonaldehyde and 1,3-butadiene and in the low-temperature oxidation of carbon monoxide. In-depth characterization of their structural and electronic properties by transmission electron microscopy (TEM), electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS) was aimed at disclosing the nature of the active sites controlling the hydrogenation and oxidation reactions. The structural characteristics such as mean particle size, size distribution and dispersion depend both on the synthetic method employed and the nature of the support. For extremely small gold particles on titania and zirconia (1.1 and 1.4 nm mean size), conduction electron spin resonance of the metal and paramagnetic F-centers (trapped electrons in oxygen vacancies) of the support were observed. The marked structure-sensitivity observed for hydrogenation properties with decreasing particle size may be attributed to structural and electronic properties due to the quantum-size effect of sufficiently small gold particles. Furthermore, the adaptability of gold particles in coatings is demonstrated for a microchannel reactor. (C) 2002 Elsevier Science B.V. All rights reserved.
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页码:63 / 78
页数:16
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