Supported gold catalysts for selective hydrogenation of 1,3-butadiene in the presence of an excess of alkenes

被引:126
作者
Hugon, Antoine [1 ]
Delannoy, Laurent [1 ]
Louis, Catherine [1 ]
机构
[1] Univ Paris 06, Lab React Surface, UMR7609, CNRS, F-75252 Paris 05, France
关键词
gold; ceria; titania; alumina; zirconia; reducibility; hydrogenation; butadiene; propene; butene; DRIFTS; TPR; TEM; catalysis;
D O I
10.1007/BF03216590
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Supported gold catalysts were investigated in the selective gas phase hydrogenation of 1,3-butadiene in an excess of propene (0.3% butadiene, 30% propene and 20% hydrogen), in order to simulate the process required for the purification of industrial alkenes streams to prevent poisoning of the polymerisation catalysts used for polyalkene production. Gold catalysts containing small gold particles (between 2 to 5 nm in average) are less active than commercial palladium catalysts, but they are much more selective. Under our experimental conditions, 100% of butadiene can be converted at similar to 170 degrees C into 100% butenes with 1-butene as the main product, and with only very small amount of alkanes formed (similar to 100 ppm). The absence or presence of propene does not drastically modify the rate of hydrogenation of butadiene. Parameters directly related to the nature of the gold catalysts were also investigated. For a given preparation method (deposition-precipitation with urea (DPU)), gold particle size and gold loading, the nature of the oxide support (alumina, titania, zirconia, ceria) does not influence the gold reactivity. The variations of gold particle size and gold loading do not induce changes in the TOF (expressed per surface gold atoms). The method of preparation has an influence when it leaves chlorine in the samples (impregnation in excess of solution and anionic adsorption). In such a case, the gold catalysts are less active.
引用
收藏
页码:127 / 138
页数:12
相关论文
共 47 条
[1]   Probing the factors affecting structure and activity of the Au/CeO2 system in total and preferential oxidation of CO [J].
Arena, F ;
Famulari, P ;
Trunfio, G ;
Bonura, G ;
Frusteri, F ;
Spadaro, L .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 66 (1-2) :81-91
[2]   Nature of Cl bonding on the Au(111) surface: Evidence of a mainly covalent interaction [J].
Baker, Thomas A. ;
Friend, Cynthia M. ;
Kaxiras, Efthimios .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (12) :3720-+
[3]  
Bergeret G., 1997, Handb. Heterog.Catal, V2, P439
[4]   FTIR study of the low-temperature water-gas shift reaction on Au/Fe2O3 and Au/TiO2 catalysts [J].
Boccuzzi, F ;
Chiorino, A ;
Manzoli, M ;
Andreeva, D ;
Tabakova, T .
JOURNAL OF CATALYSIS, 1999, 188 (01) :176-185
[5]  
BOCCUZZI F, 2000, SURF SCI, V942, P454
[6]  
BOND GC, 1973, J CHEM SOC CHEM COMM, P444
[7]  
Bond GC, 2006, CATALY SCI SER, V6, P1, DOI 10.1142/9781860948954
[8]   CATALYSIS BY GROUP IB METALS .1. REACTION OF BUTA-1,3-DIENE WITH HYDROGEN AND WITH DEUTERIUM CATALYZED BY ALUMINA-SUPPORTED GOLD [J].
BUCHANAN, DA ;
WEBB, G .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1975, 71 (01) :134-144
[9]   Hydrogen chemisorption on Al2O3-supported gold catalysts [J].
Bus, E ;
Miller, JT ;
van Bokhoven, JA .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (30) :14581-14587
[10]   Acetylene hydrogenation on Au-based catalysts [J].
Choudhary, TV ;
Sivadinarayana, C ;
Datye, AK ;
Kumar, D ;
Goodman, DW .
CATALYSIS LETTERS, 2003, 86 (1-3) :1-8