A study of K-promoted MoP-SiO2 catalysts for synthesis gas conversion

被引:41
作者
Zaman, Sharif F. [1 ]
Smith, Kevin J. [1 ]
机构
[1] Univ British Columbia, Dept Chem & Biol Engn, Vancouver, BC V6T 1Z3, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
Synthesis gas; Gas-to-liquids; MoP; Catalyst; Ethanol; Acetaldehyde; Acetone; C2+ oxygenates; Alcohols; MIXED ALCOHOLS SYNTHESIS; TRANSITION-METAL PHOSPHIDES; SILICA-SUPPORTED MOLYBDENUM; DENSITY-FUNCTIONAL THEORY; CO HYDROGENATION; BETA-MO2C CATALYSTS; OXYGENATE SYNTHESIS; RH CATALYSTS; SYNGAS; POTASSIUM;
D O I
10.1016/j.apcata.2010.01.046
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 conversion of synthesis gas to oxygenated hydrocarbons over a series of K-promoted MoP-SiO2 catalysts, is reported. Catalysts with 5, 10, and 15 wt% MoP on SiO2 and promoted with 1 and 5 wt% K. were prepared, characterized and tested at 548 K, 8.27 MPa and a H-2:CO = 1. An increase in CO conversion was observed with increased MOP and K loading and the highest oxygenate space time yield of 147.2 mg g cat(-1) h(-1) was obtained over the 5 wt% K-15 wt% MoP-SiO2 catalyst. CH4 was produced with high selectivity (29-40 C atom%) over the un-promoted MOP catalysts, but with the addition of K. the CH4 selectivity was suppressed and the C2+ oxygenated product selectivity increased as the surface K/Mo atom ratio increased, up to a maximum at a K/Mo ratio of 3.2. The highest selectivity towards C2+ oxygenates (76.6 C atom%) and lowest selectivity towards CH4 (9.7 C atom%) occurred on the 5 wt% K-10 wt% MoP-SiO2 catalyst. The major oxygenates in the product were acetaldehyde, acetone and ethanol. In all cases, catalyst selectivity to methanol was low (<5.0 atom%). The product distribution obtained over the K-MoP-SiO2 catalysts was distinct from that reported on other Mo-based catalysts. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:59 / 68
页数:10
相关论文
共 51 条
[1]   The effect of cobalt addition to bulk MoP and Ni2P catalysts for the hydrodesulfurization of 4,6-dimethyldibenzothiophene [J].
Abu, Ibrahim I. ;
Smith, Kevin J. .
JOURNAL OF CATALYSIS, 2006, 241 (02) :356-366
[2]   SYNTHESIS GAS CONVERSION OVER SUPPORTED RHODIUM AND RHODIUM-IRON CATALYSTS [J].
BHASIN, MM ;
BARTLEY, WJ ;
ELLGEN, PC ;
WILSON, TP .
JOURNAL OF CATALYSIS, 1978, 54 (02) :120-128
[3]   High temperature calcined K-MoO3/γ-Al2O3 catalysts for mixed alcohols synthesis from syngas:: Effects of Mo loadings [J].
Bian, GZ ;
Fan, L ;
Fu, YL ;
Fujimoto, K .
APPLIED CATALYSIS A-GENERAL, 1998, 170 (02) :255-268
[4]   Mechanism of C2+ oxygenate synthesis on Rh catalysts [J].
Chuang, SSC ;
Stevens, RW ;
Khatri, R .
TOPICS IN CATALYSIS, 2005, 32 (3-4) :225-232
[5]   Alumina-supported molybdenum phosphide hydroprocessing catalysts [J].
Clark, PA ;
Oyama, ST .
JOURNAL OF CATALYSIS, 2003, 218 (01) :78-87
[6]   Effect of H2/CO ratio and temperature on methane selectivity in the synthesis of ethanol on Rh-based catalysts [J].
Egbebi, Adefemi ;
Spivey, James J. .
CATALYSIS COMMUNICATIONS, 2008, 9 (14) :2308-2311
[7]  
Ellgen P.C., 1979, Advances in Chemistry, V178, P147
[8]   The study of reactions influencing the biomass steam gasification process [J].
Franco, C ;
Pinto, F ;
Gulyurtlu, I ;
Cabrita, I .
FUEL, 2003, 82 (07) :835-842
[9]   CO hydrogenation on lanthana and vanadia doubly promoted Rh/SiO2 catalysts [J].
Gao, Jia ;
Mo, Xunhua ;
Chien, Andrew Chang-Yin ;
Torres, Walter ;
Goodwin, James G., Jr. .
JOURNAL OF CATALYSIS, 2009, 262 (01) :119-126
[10]  
GEORGE WH, 2006, CHEM REV CHEMINFORM