Acetylene hydrogenation over Ni-Si-Al mixed oxides prepared by sol-gel technique

被引:68
作者
Guimon, C
Auroux, A
Romero, E
Monzon, A
机构
[1] Univ Pau & Pays Adour, Lab Physicochim Mol, CNRS, UMR 5624, F-64053 Pau 9, France
[2] Inst Rech Catalyse, F-69626 Villeurbanne, France
[3] Univ Zaragoza, Fac Sci, Dept Chem Engn, E-50009 Zaragoza, Spain
关键词
sol-gel Ni catalysts; acetylene hydrogenation; coking; TPR; TPO; XPS;
D O I
10.1016/S0926-860X(03)00318-1
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
The effect of the support (here silica and silica-alumina) and of the composition of Ni-based hydrogenation catalysts, elaborated by sol-gel method, on their physico-chemical characteristics and on their activity and selectivity (towards ethylene) for acetylene hydrogenation has been studied with the help of temperature programmed reduction (TPR) and oxidation (TPO), X-ray photoelectron spectroscopy (XPS) and reaction tests (acetylene to ethylene hydrogenation). These techniques have shown the existence of two different types of sites. Firstly, the hydrogenolytic (naked) metallic centres, corresponding to nickel without (or little) interaction with the support, are responsible for a large part of the coke and are active for side-reactions. Secondly, the hydrogenating sites correspond to nickel in interaction with the support and are active for the main reaction. Three types of coke have been detected: filaments, amorphous coke, and partially hydrogenated carbons strongly adsorbed on the surface. The latter are facilitated by the acidity of the silica-alumina. Because the metal-support interactions related to a better dispersion of reduced nickel, silica-alumina-based catalysts produce a much smaller amount of coke than silica-based catalysts. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:199 / 214
页数:16
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