Creation of the active site for methanol synthesis on a Cu/SiO2 catalyst

被引:41
作者
Fujitani, T [1 ]
Matsuda, T
Kushida, Y
Ogihara, S
Uchijima, T
Nakamura, J
机构
[1] Natl Inst Resources & Environm, Ibaraki, Osaka 305, Japan
[2] Res Inst Innovat Technol Earth, Soura Ku, Kyoto 305, Japan
[3] Univ Tsukuba, Inst Sci Mat, Ibaraki, Osaka 305, Japan
关键词
methanol synthesis; Cu/ZnO catalyst; hydrogenation of CO2; role of Zn; in situ FT-IR;
D O I
10.1023/A:1019069708459
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 ZnO/SiO2 in a physical mixture of Cu/SiO2 and ZnO/SiO2 on methanol synthesis from CO2 and H-2 was studied to clarify the role of ZnO in Cu/ZnO-based catalysts. An active Cu/SiO2 was prepared by the following procedure: the Cu/SiO2 and ZnO/SiO2 catalysts with a different SiO2 particle size were mixed and reduced with H-2 at 523-723 K, and the Cu/SiO2 was then separated from the mixture using a sieve. The methanol synthesis activity of the Cu/SiO2 catalyst increased with the reduction temperature and was in fairly good agreement with that previously obtained for the physical mixture of Cu/SiO2 and ZnO/SiO2. These results indicated that the active site for methanol synthesis was created on the Cu/SiO2 upon reduction of the physical mixture with H-2. It was also found that ZnO itself had no promotional effect on the methanol synthesis activity except for the role of ZnO to create the active site. The active site created on the Cu/SiO2 catalyst was found not to promote the formation of formate from CO2 and H-2 on the Cu surface based on in situ FT-IR measurements. A special formate species unstable at 523 K with an OCO asymmetric peak at similar to 1585 cm(-1) was considered to be adsorbed on the active site.
引用
收藏
页码:175 / 179
页数:5
相关论文
共 30 条
[1]   MECHANISM AND KINETICS OF METHANOL SYNTHESIS ON ZINC-OXIDE [J].
BOWKER, M ;
HOUGHTON, H ;
WAUGH, KC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1981, 77 :3023-3036
[2]   THE MECHANISM OF METHANOL SYNTHESIS ON COPPER-ZINC OXIDE ALUMINA CATALYSTS [J].
BOWKER, M ;
HADDEN, RA ;
HOUGHTON, H ;
HYLAND, JNK ;
WAUGH, KC .
JOURNAL OF CATALYSIS, 1988, 109 (02) :263-273
[3]   SYNERGY AT A DISTANCE IN THE SYNTHESIS OF METHANOL OVER COPPER CATALYSTS [J].
Burch, R. ;
Chappell, R. J. ;
Golunski, S. E. .
CATALYSIS LETTERS, 1988, 1 (12) :439-443
[4]   THE ROLE OF COPPER AND ZINC-OXIDE IN METHANOL SYNTHESIS CATALYSTS [J].
BURCH, R ;
GOLUNSKI, SE ;
SPENCER, MS .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1990, 86 (15) :2683-2691
[5]   SYNERGY BETWEEN COPPER AND ZINC-OXIDE DURING METHANOL SYNTHESIS - TRANSFER OF ACTIVATING SPECIES [J].
BURCH, R ;
CHAPPELL, RJ ;
GOLUNSKI, SE .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1989, 85 :3569-3578
[6]   Wetting/non-wetting phenomena during catalysis: evidence from in situ on-line EXAFS studies of Cu-based catalysts [J].
Clausen, Bjerne S. ;
Schiotz, Jakob ;
Grabaek, Lars ;
Ovesen, Charlotte V. ;
Jacobsen, Karsten W. ;
Norskov, Jens K. ;
Topsoe, Henrik .
TOPICS IN CATALYSIS, 1994, 1 (3-4) :367-376
[7]   NEW INSIGHTS INTO THE KINETICS OF FORMIC-ACID DECOMPOSITION ON COPPER SURFACES [J].
DUBOIS, LH ;
ELLIS, TH ;
ZEGARSKI, BR ;
KEVAN, SD .
SURFACE SCIENCE, 1986, 172 (02) :385-397
[8]   METHANOL SYNTHESIS FROM CO2 AND H-2 OVER A ZNO CATALYST - EFFECT OF THE PRETREATMENT WITH CO-H-2 UPON THE REACTION [J].
FUJITA, S ;
ITO, H ;
TAKEZAWA, N .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1993, 66 (10) :3094-3096
[9]   Mechanisms of methanol synthesis from carbon dioxide and from carbon monoxide at atmospheric pressure over Cu/ZnO [J].
Fujita, S ;
Usui, M ;
Ito, H ;
Takezawa, N .
JOURNAL OF CATALYSIS, 1995, 157 (02) :403-413
[10]   METHANOL SYNTHESIS FROM CARBON-DIOXIDE AT ATMOSPHERIC-PRESSURE OVER CU/ZNO CATALYST - ROLE OF METHOXIDE SPECIES FORMED ON ZNO SUPPORT [J].
FUJITA, S ;
USUI, M ;
OHARA, E ;
TAKEZAWA, N .
CATALYSIS LETTERS, 1992, 13 (04) :349-358