Oxygen adsorption on Au/Al2O3 catalysts and relation to the catalytic oxidation of ethylene glycol to glycolic acid

被引:81
作者
Berndt, H [1 ]
Pitsch, I [1 ]
Evert, S [1 ]
Struve, K [1 ]
Pohl, MM [1 ]
Radnik, J [1 ]
Martin, A [1 ]
机构
[1] Inst Angew Chem Berlin Adlershof EV, ACA, D-12489 Berlin, Germany
关键词
gold catalysts; oxygen chemisorption; hydrogen titration; TEM; XPS; selective oxidation; ethylene glycol; glycolic acid; particle; size influence;
D O I
10.1016/S0926-860X(02)00575-6
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
Static oxygen adsorption and hydrogen pulse titration of chemisorbed oxygen were checked and successfully used as tools for characterisation of the dispersity and surface area of Au/Al2O3 catalysts tested in the oxidation of ethylene glycol. Using a stoichiometry of Au-s:O = 2 a good agreement was obtained between the average gold particle size calculated from oxygen chemisorption results and the particle size preferentially observed by TEM. A correlation of the catalytic activity with the oxygen adsorption of Au/Al2O3 catalysts having different An dispersity and content showed a steady increase of the rate of the glycolic acid formation with increasing oxygen chemisorption and Au surface area, respectively. No differences in the selectivity of the reaction were observed with low- and high-disperse Au/Al2O3 catalysts, a selectivity to glycolic acid higher than 95% was obtained on all the samples. Therefore, we could clearly demonstrate that the selective oxidation of ethylene glycol to glycolic acid is not a structure-sensitive reaction, i.e. this reaction is not restricted to a defined gold particle size, as for example in the epoxidation of propylene over Au/TiO2. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:169 / 179
页数:11
相关论文
共 21 条
[1]   Selective oxidation of glycerol to glyceric acid using a gold catalyst in aqueous sodium hydroxide [J].
Carrettin, S ;
McMorn, P ;
Johnston, P ;
Griffin, K ;
Hutchings, GJ .
CHEMICAL COMMUNICATIONS, 2002, (07) :696-697
[2]   Characterizations of alumina-supported gold with temperature-programmed reduction [J].
Chang, CK ;
Chen, YJ ;
Yeh, CT .
APPLIED CATALYSIS A-GENERAL, 1998, 174 (1-2) :13-23
[3]   Deposition of highly dispersed gold on alumina support [J].
Chen, YJ ;
Yeh, CT .
JOURNAL OF CATALYSIS, 2001, 200 (01) :59-68
[4]   CHEMISORPTION OF OXYGEN, WATER AND SELECTED HYDROCARBONS ON (111) AND STEPPED GOLD SURFACES [J].
CHESTERS, MA ;
SOMORJAI, GA .
SURFACE SCIENCE, 1975, 52 (01) :21-28
[5]   Properties of adsorbed oxygen on Au/SiO2 [J].
Choi, KH ;
Coh, BY ;
Lee, HI .
CATALYSIS TODAY, 1998, 44 (1-4) :205-213
[6]   DECOMPOSITION OF NITROUS OXIDE CATALYSED BY PALLADIUM-GOLD ALLOY WIRES [J].
ELEY, DD ;
KNIGHTS, CF .
PROCEEDINGS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL AND PHYSICAL SCIENCES, 1966, 294 (1436) :1-+
[7]   OXYGEN-CHEMISORPTION ON SUPPORTED GOLD [J].
FUKUSHIMA, T ;
GALVAGNO, S ;
PARRAVANO, G .
JOURNAL OF CATALYSIS, 1979, 57 (01) :177-182
[8]   HEATS OF ADSORPTION OF OXYGEN ON NICKEL, PLATINUM AND SILVER [J].
GONZALEZ, OD ;
PARRAVANO, G .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1956, 78 (18) :4533-4537
[9]   Size- and support-dependency in the catalysis of gold [J].
Haruta, M .
CATALYSIS TODAY, 1997, 36 (01) :153-166
[10]   The reaction of molecular oxygen with silver at technical catalytic conditions: Bulk structural consequences of a gas-solid interface reaction [J].
Herein, D ;
Nagy, A ;
Schubert, H ;
Weinberg, G ;
Kitzelmann, E ;
Schlogl, R .
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS, 1996, 197 :67-96