FTIR studies of CO adsorption on Al2O3- and SiO2-supported Ru catalysts

被引:250
作者
Chin, SY [1 ]
Williams, CT [1 ]
Amiridis, MD [1 ]
机构
[1] Univ S Carolina, Dept Chem Engn, Columbia, SC 29208 USA
关键词
D O I
10.1021/jp053908q
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 [物理化学]; 081704 [应用化学];
摘要
The adsorption of CO on Al2O3- and SiO2-supported Ru catalysts has been investigated through FTIR spectroscopy. Deconvolution of the spectra obtained reveals the presence of 11 distinct bands in the case of Ru/Al2O3 and 10 bands in the case of Ru/SiO2, which were assigned to different carbonyl species adsorbed on reduced as well as partially oxidized Ru sites. Although most of these bands on both supports are similar, they exhibit substantial differences in terms of stability. In general, the analogous CO species on Ru/Al2O3 are adsorbed stronger than those on Ru/SiO2, with the most stable species observed being a dicarbonyl adsorbed on metallic Ru (i.e., Ru-0(CO)(2)). Following sintering of the Ru, the ratio of multicarbonyl to monocarborlyl adsorption is reduced substantially because of the lack of isolated sites or small Ru clusters that enable the formation of multicarbonyl species via oxidative disruption. Finally, in the presence of O-2, the main features observed correspond to nionocarbonyl, dicarbonyl, and tricarbonyl species adsorbed on partially oxidized Run+. The intensities of all bands decrease drastically at temperatures above 210 degrees C because of the onset of CO oxidation, which results in substantially reduced Surface coverage.
引用
收藏
页码:871 / 882
页数:12
相关论文
共 40 条
[1]
ABHIVANTANAPORN P, 1984, J CATAL, V90, P119
[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]
INFRARED-SPECTRA AND REACTIVITY OF DI-MU-HALOBIS(HALOTRICARBONYLRUTHENIUM) [J].
BENEDETTI, E ;
BRACA, G ;
SBRANA, G ;
SALVETTI, F ;
GRASSI, B .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1972, 37 (02) :361-+
[4]
CATALYTIC AND STRUCTURAL-PROPERTIES OF RUTHENIUM BIMETALLIC CATALYSTS - EFFECTS OF PRETREATMENT ON THE BEHAVIOR OF VARIOUS RU/AL2O3 CATALYSTS IN ALKANE HYDROGENOLYSIS [J].
BOND, GC ;
SLAA, JC .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1995, 96 (02) :163-173
[5]
STUDIES ON RUTHENIUM CATALYSTS .4. HYDROGENOLYSIS OF N-BUTANE ON RU/AL2O3 CATALYST-DEPENDENCE OF REACTION-KINETICS ON PARTICLE-SIZE AND ON PRETREATMENT [J].
BOND, GC ;
SLAA, JC .
JOURNAL OF MOLECULAR CATALYSIS, 1994, 89 (1-2) :221-228
[6]
Bossi A., 1978, STUD SURF SCI CATAL, V3, P405
[7]
INFRARED STUDY OF ADSORPTION OF CARBON-MONOXIDE ON REDUCED AND OXIDIZED FORMS OF SILICA SUPPORTED RUTHENIUM [J].
BROWN, MF ;
GONZALEZ, RD .
JOURNAL OF PHYSICAL CHEMISTRY, 1976, 80 (15) :1731-1735
[8]
CO CHEMISORPTION ON RU/SIO2 - THE INFLUENCE OF COADSORBATES [J].
CHEN, HW ;
ZHONG, Z ;
WHITE, JM .
JOURNAL OF CATALYSIS, 1984, 90 (01) :119-126
[9]
Preferential oxidation of CO under excess H2 conditions over Ru catalysts [J].
Chin, SY ;
Alexeev, OS ;
Amiridis, MD .
APPLIED CATALYSIS A-GENERAL, 2005, 286 (02) :157-166
[10]
CATALYTIC AND STRUCTURAL-PROPERTIES OF RUTHENIUM BIMETALLIC CATALYSTS - PREPARATION AND CHARACTERIZATION [J].
COQ, B ;
CRABB, E ;
WARAWDEKAR, M ;
BOND, GC ;
SLAA, JC ;
GALVAGNO, S ;
MERCADANTE, L ;
RUIZ, JG ;
SIERRA, MCS .
JOURNAL OF MOLECULAR CATALYSIS, 1994, 92 (01) :107-121