Water gas shift reaction kinetics under noncatalytic conditions in supercritical water

被引:85
作者
Sato, T
Kurosawa, S
Smith, RL
Adschiri, T
Arai, K
机构
[1] Natl Inst Adv Ind Sci & Technol, Supercrit Fluid Res Ctr, Sendai, Miyagi 9838551, Japan
[2] Tohoku Univ, Dept Chem Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan
[3] Tohoku Univ, Res Ctr Supercrit Fluid Technol, Aoba Ku, Sendai, Miyagi 9808579, Japan
[4] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Aoba Ku, Sendai, Miyagi 9808577, Japan
关键词
supercritical water; water gas shift reaction; carbon monoxide; hydrogen; kinetics;
D O I
10.1016/S0896-8446(03)00049-4
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
The kinetics of the water gas shift reaction was studied under noncatalytic conditions in supercritical water at CO/H2O ratios of 0.03 and at temperatures from 653 to 713 K. The selectivities of CO2 and hydrogen were almost equal and did not change with pressure at 673 K. The increase of pressure and water density sensitively promoted the reaction at 653 K from 25 to 30 MPa whereas the pressure and water density did not seem to affect the rate constant at 673 K from 10 to 30 MPa. The first order rate constant for CO conversion was k = 10(5.58+/-1.38) exp(-1.16 +/- 0.19 x 10(5)/RT) /s at 10-59.6 MPa and 653-866 K. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:113 / 119
页数:7
相关论文
共 15 条
[1]   Biomass gasification in supercritical water [J].
Antal, MJ ;
Allen, SG ;
Schulman, D ;
Xu, XD ;
Divilio, RJ .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (11) :4040-4053
[2]   Catalytic oxidation in supercritical water [J].
Ding, ZY ;
Frisch, MA ;
Li, LX ;
Gloyna, EF .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1996, 35 (10) :3257-3279
[3]   AQUEOUS CATALYST SYSTEMS FOR THE WATER GAS SHIFT REACTION .1. COMPARATIVE CATALYST STUDIES [J].
ELLIOTT, DC ;
SEALOCK, LJ .
INDUSTRIAL & ENGINEERING CHEMISTRY PRODUCT RESEARCH AND DEVELOPMENT, 1983, 22 (03) :426-431
[4]  
Ertl, 1997, HDB HETEROGENEOUS CA, DOI DOI 10.1002/9783527619474
[5]   KINETICS AND MECHANISMS OF THE 2 OPPOSING REACTIONS OF THE EQUILIBRIUM CO + H2O = CO2 + H21 [J].
GRAVEN, WM ;
LONG, FJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1954, 76 (10) :2602-2607
[6]   OXIDATION AND HYDROTHERMOLYSIS OF HYDROCARBONS IN SUPERCRITICAL WATER AT HIGH-PRESSURES [J].
HIRTH, T ;
FRANCK, EU .
BERICHTE DER BUNSEN-GESELLSCHAFT-PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1993, 97 (09) :1091-1098
[7]   CARBON-MONOXIDE OXIDATION IN SUPERCRITICAL WATER - THE EFFECTS OF HEAT-TRANSFER AND THE WATER GAS SHIFT REACTION ON OBSERVED KINETICS [J].
HOLGATE, HR ;
WEBLEY, PA ;
TESTER, JW ;
HELLING, RK .
ENERGY & FUELS, 1992, 6 (05) :586-597
[8]   Stationary and transient kinetics of the high temperature water-gas shift reaction [J].
Keiski, RL ;
Salmi, T ;
Niemisto, P ;
Ainassaari, J ;
Pohjola, VJ .
APPLIED CATALYSIS A-GENERAL, 1996, 137 (02) :349-370
[9]  
KROSCHWITZ JI, 1991, ENCY CHEM TECHNOLOGY
[10]  
Lemmon E.W., 2001, THERMOPHYSICAL PROPE