PdZnAl catalysts for the reactions of water-gas-shift, methanol steam reforming, and reverse-water-gas-shift

被引:60
|
作者
Dagle, R. A. [1 ]
Platon, A. [1 ]
Palo, D. R. [1 ]
Datye, A. K. [2 ]
Vohs, J. M. [3 ]
Wang, Y. [1 ]
机构
[1] Pacific NW Natl Lab, Richland, WA 99354 USA
[2] Univ New Mexico, Dept Chem & Nucl Engn, Albuquerque, NM 87131 USA
[3] Univ Penn, Dept Chem & Bimol Engn, Philadelphia, PA 19104 USA
关键词
PdZnAl catalyst; water-gas-shift (WGS); methanol steam reforming; reverse-water-gas-shift; fuel processing;
D O I
10.1016/j.apcata.2008.03.005
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
Pd/ZnO/Al2O3 catalysts were studied for water-gas-shift (WGS), methanol steam reforming, and reverse-water-gas-shift (RWGS) reactions. WGS activity was found to be dependent on the Pd:Zn ratio with a maximum activity obtained at approximately 0.50, which was comparable to that of a commercial Pt-based catalyst. The catalyst stability was demonstrated for 100 h time-on-stream at a temperature of 360 degrees C without evidence of metal sintering. WGS reaction rates were approximately 1st order with respect to CO concentration, and kinetic parameters were determined to be E-a = 58.3 kJ mol(-1) and k(o) = 6.1 X 10(7) mol(-1). During methanol steam reforming, the CO selectivities were observed to be lower than the calculated equilibrium values over a range of temperatures and steam/carbon ratios studied while the reaction rate constants were approximately of the same magnitude for both WGS and methanol steam reforming. These results indicate that although Pd/ZnO/Al2O3 are active WGS catalysts, WGS is not involved in methanol steam reforming. RWGS rate constants are on the order of about 20 times lower than that of methanol steam reforming, suggesting that RWGS reaction could be one of the sources for small amount of CO formation in methanol steam reforming. (c) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:63 / 68
页数:6
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