Modifications of surface properties of a H2-treated RuS2/SiO2 catalyst:: A parallel between low-temperature COFTIR spectroscopy and model reactions

被引:14
作者
Berhault, G
Maugé, F
Lavalley, JC
Lacroix, M
Breysse, M
机构
[1] Univ Caen, ISMRA, Catalyse & Spectrochim Lab, F-14050 Caen, France
[2] Inst Rech Catalyse, F-69629 Villeurbanne, France
[3] Univ Paris 06, Lab React Surface, F-75252 Paris 05, France
关键词
D O I
10.1006/jcat.1999.2715
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 silica-supported ruthenium sulfide catalyst was progressively reduced by hydrogen at increasing temperatures (423-673 K). The resulting modification of the surface properties was characterized by low-temperature CO adsorption FTIR spectroscopy and by test reactions such as CH3SH condensation and 1-butene hydrogenation. On the nonreduced catalyst, CO adsorption spectra showed the presence of bands, indicating various CO forms on Ru sites in a sulfur-rich environment. When sulfur was progressively removed from the ruthenium sulfide phase, the number of coordinatively unsaturated Ru sites increased with the simultaneous formation of metallic Ru microdomains. A comparison of measurements of adsorption and catalytic activity showed that a rich sulfur environment was needed for the condensation of CH3SH to CH3SCH3, a reaction that required acidic sites, while butene hydrogenation required highly depleted Ru sites. These results show that, upon reduction, RuS2 became less acidic and increasingly more metallic. (C) 2000 Academic Press.
引用
收藏
页码:431 / 437
页数:7
相关论文
共 40 条
[1]   IR-SPECTROSCOPIC DETECTION OF LEWIS ACID SITES ON AL2O3 USING ADSORBED CO - CORRELATION WITH AL-OH GROUP REMOVAL [J].
BALLINGER, TH ;
YATES, JT .
LANGMUIR, 1991, 7 (12) :3041-3045
[2]   REACTIVITY OF SURFACE INTERMEDIATES DERIVED FROM AL2O3-SUPPORTED RU3(CO)12 IN THE CO+H-2 REACTION [J].
BECK, A ;
DOBOS, S ;
GUCZI, L .
INORGANIC CHEMISTRY, 1988, 27 (18) :3220-3226
[3]   Characterization of acid-base paired sites on silica-supported RuS2 by infrared spectroscopy and methyl mercaptan condensation reaction [J].
Berhault, G ;
Lacroix, M ;
Breysse, M ;
Mauge, F ;
Lavalley, JC ;
Qu, LL .
JOURNAL OF CATALYSIS, 1997, 170 (01) :37-45
[4]   Characterization of acidic sites of silica-supported transition metal sulfides by pyridine and 2,6 dimethylpyridine adsorption:: Relation to activity in CH3SH condensation [J].
Berhault, G ;
Lacroix, M ;
Breysse, M ;
Mauge, F ;
Lavalley, JC ;
Nie, H ;
Qu, LL .
JOURNAL OF CATALYSIS, 1998, 178 (02) :555-565
[5]   CNDO MODEL OF CARBON-MONOXIDE CHEMISORBED ON NICKEL [J].
BLYHOLDER, G .
JOURNAL OF PHYSICAL CHEMISTRY, 1975, 79 (07) :756-761
[6]  
BURKHARDT I, 1991, STUD SURF SCI CATAL, V69, P215
[7]   Spectroscopic characterization of the acid properties of metal oxide catalysts [J].
Busca, G .
CATALYSIS TODAY, 1998, 41 (1-3) :191-206
[8]  
Davydov A. A., 1990, INFRARED SPECTROSCOP
[9]   IR STUDY OF NO AND CO ADSORPTION ON A SILICA-SUPPORTED RU CATALYST [J].
DAVYDOV, AA ;
BELL, AT .
JOURNAL OF CATALYSIS, 1977, 49 (03) :332-344
[10]   USE OF CO AS PROBE MOLECULE FOR CHARACTERIZATION OF MIXED RU-NI SULFIDE PHASES SUPPORTED OVER ALUMINA [J].
DELOSREYES, JA ;
VRINAT, M ;
BREYSSE, M ;
MAUGE, F ;
LAVALLEY, JC .
CATALYSIS LETTERS, 1992, 13 (03) :213-219