Methanol synthesis pathway over Cu/ZrO2 catalysts:: a time-resolved DRIFT 13C-labelling experiment

被引:33
作者
Ortelli, EE
Weigel, JM
Wokaun, A [1 ]
机构
[1] Paul Scherrer Inst, CH-5232 Villigen, Switzerland
[2] ETH Zentrum, Swiss Fed Inst Technol, Dept Chem Engn & Ind Chem, CH-8092 Zurich, Switzerland
关键词
methanol synthesis; Cu/ZrO2; DRIFT; C-13-labelling experiments;
D O I
10.1023/A:1019032022881
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
To provide additional evidence on the synthesis path of methanol over Cu/ZrO2 catalysts, a three-step in situ experiment was performed in a DRIFT cell. C-13-labelled as well as common C-12 paraformaldehyde and formic acid were adsorbed and subsequently hydrogenated under reaction conditions (0.5 MPa and 423 K). It was found that methanol was generated exclusively from the eta(2)-H2CO intermediate, not from adsorbed surface formate. Furthermore, the intermediacy of CO32- in the reverse/water-gas shift reaction was shown.
引用
收藏
页码:41 / 48
页数:8
相关论文
共 19 条
[1]   AN INFRARED SPECTROSCOPIC STUDY ON THE MECHANISM OF METHANOL FORMATION FROM CO AND H-2 OVER ZIRCONIA [J].
ABE, H ;
MARUYA, K ;
DOMEN, K ;
ONISHI, T .
CHEMISTRY LETTERS, 1984, (11) :1875-1878
[2]   METHANOL SYNTHESIS FROM CO2+H2 .2. COPPER-BASED BINARY AND TERNARY CATALYSTS [J].
AMENOMIYA, Y .
APPLIED CATALYSIS, 1987, 30 (01) :57-68
[3]   In-situ infrared study of methanol synthesis from H-2/CO2 over Cu/SiO2 and Cu/ZrO2/SiO2 [J].
Fisher, IA ;
Bell, AT .
JOURNAL OF CATALYSIS, 1997, 172 (01) :222-237
[4]   Effects of zirconia promotion on the activity of Cu/SiO2 for methanol synthesis from CO/H-2 and CO2/H-2 [J].
Fisher, IA ;
Woo, HC ;
Bell, AT .
CATALYSIS LETTERS, 1997, 44 (1-2) :11-17
[5]   HYDROGENATION OF CARBON-DIOXIDE OVER SILVER PROMOTED COPPER/ZIRCONIA CATALYSTS [J].
FROHLICH, C ;
KOPPEL, RA ;
BAIKER, A ;
KILO, M ;
WOKAUN, A .
APPLIED CATALYSIS A-GENERAL, 1993, 106 (02) :275-293
[6]   CO AND CO-2 HYDROGENATION OVER METAL-OXIDES - A COMPARISON OF ZNO, TIO2 AND ZRO2 [J].
HE, MY ;
WHITE, JM ;
EKERDT, JG .
JOURNAL OF MOLECULAR CATALYSIS, 1985, 30 (03) :415-430
[7]   TEMPERATURE-PROGRAMMED STUDIES OF THE ADSORPTION OF SYNTHESIS GAS ON ZIRCONIUM DIOXIDE [J].
HE, MY ;
EKERDT, JG .
JOURNAL OF CATALYSIS, 1984, 87 (01) :238-254
[8]  
KOPPEL RA, 1991, J CHEM SOC FARADAY T, V87, P2821
[9]   OPTIMIZATION OF SAMPLE PACKING IN DIFFUSE-REFLECTANCE INFRARED-SPECTROSCOPY [J].
KRIVACSY, Z ;
HLAVAY, J .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1994, 50 (01) :49-55