ZNO-CR2O3+ZSM-5 CATALYST WITH VERY-LOW ZN/CR RATIO FOR THE TRANSFORMATION OF SYNTHESIS GAS TO HYDROCARBONS

被引:67
作者
SIMARD, F
SEDRAN, UA
SEPULVEDA, J
FIGOLI, NS
DELASA, HI
机构
[1] UNIV WESTERN ONTARIO,FAC ENGN SCI,CTR CHEM REACTOR ENGN,DEPT CHEM & BIOCHEM ENGN,LONDON,ON N6A 5B9,CANADA
[2] CHEVRON RES & TECHNOL CO,DIV ORONITE TECHNOL,RICHMOND,CA 94802
[3] UNL,CONICET,FIQ,INCAPE,RA-3000 SANTA FE,ARGENTINA
关键词
CATALYST CHARACTERIZATION (XRD; DTA; BET; TPR; IR; XPS); HYDROCARBONS; SYNGAS CONVERSION; ZINC OXIDE CHROMIUM OXIDE; ZEOLITES; ZSM-5;
D O I
10.1016/0926-860X(94)00275-4
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
Three Zn-Cr mixed oxide plus ZSM-5 compound catalysts with different compositions covering a wide range of Zn/Cr atomic ratios (0.064 to 1.913), aimed at the direct conversion of synthesis gas into hydrocarbons, were tested under different experimental conditions: temperature ranged from 356 to 410 degrees C, pressure from 3.60 to 4.49 MPa and space velocity from 0.2 to 3.0 mmol reactants/(g(cat) min). Reaction products included carbon dioxide, water and hydrocarbons with methanol conversion (through which hydrocarbons are formed) being complete. The catalyst with the least content of zinc gave the highest yields of liquid hydrocarbons (up to 74% of total hydrocarbons). Different crystalline phases (ZnO, ZnCr2O4 and Cr2O3) were found in the methanol synthesis component as a function of Zn/Cr ratio, The low Zn/Cr catalyst was characterized by X-ray diffraction, differential thermal analysis, nitrogen adsorption, temperature-pro rammed reduction, Infrared and X-ray photoelectron spectroscopy. The only phases observed in this catalyst were ZnCr2O4 and Cr2O3. Calcination temperature had an influence in both physical and chemical catalyst properties. After calcination, Cr-VI and Cr-III species could be seen on the catalyst surface, but only Cr-III species were observed after reaction or reduction. The evidences gathered suggest that Cr2O3 is mainly responsible for methanol synthesis, while ZnCr2O4 contributes to increase the specific surface area of the catalyst and influences gas product distributions, Compound catalysts with the mixed oxide (Zn-Cr) as the methanol synthesis component showed to be more active than those with the individual (Cr or Zn) oxides.
引用
收藏
页码:81 / 98
页数:18
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