An investigation using SSITKA of Chain growth on Fe and FeMnK Fischer-Tropsch synthesis catalysts

被引:24
作者
Lohitharn, Nattaporn [1 ]
Goodwin, James G., Jr. [1 ]
机构
[1] Clemson Univ, Dept Chem & Biomol Engn, Clemson, SC 29634 USA
关键词
Fischer-Tropsch synthesis (FTS); CO hydrogenation; Steady-state isotopic transient kinetic analysis (SSITKA); Mn promotion; K promotion; Water-gas shift (WGS); Fe-based FTS catalysts; Reaction pathway; Chain growth; TRANSIENT KINETIC-ANALYSIS; IRON; METHANATION; MECHANISM;
D O I
10.1016/j.catcom.2008.11.039
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
Although FTS is a simple reaction between CO and H-2, its reaction mechanism is not straightforward since it involves a large number of surface species for the formation of a variety of products. In this study, steady-state isotopic transient kinetic analysis (SSITKA) was utilized to estimate the average surface residence times leading to CO2 and various hydrocarbon products in order to investigate chain growth and termination for hydrocarbon products formed on unpromoted and K- and Mn-promoted FeCuSiO2 catalysts. The addition of K and Mn to the Fe catalyst promoted significantly the catalytic activity of Fe but did not have a significant impact on the chain growth or chain termination steps. Instead, an increase in the concentration of active Surface intermediates leading to hydrocarbon products was the primary cause for the improved catalyst activity. Chain termination was found to be relatively fast compared to chain growth for the Fe FTS catalysts with and without K and Mn promotion, as the average surface residence times of methane, ethane, ethylene, propane and propylene showed. (c) 2008 Elsevier B.V. All rights reserved.
引用
收藏
页码:758 / 762
页数:5
相关论文
共 18 条
[1]   Slurry phase Fischer-Tropsch synthesis over manganese-promoted iron ultrafine particle catalyst [J].
Bai, L ;
Xiang, HW ;
Li, YW ;
Han, YZ ;
Zhong, B .
FUEL, 2002, 81 (11-12) :1577-1581
[2]   ON THE MECHANISM OF THE FISCHER-TROPSCH REACTION - THE CHAIN PROPAGATION STEP [J].
BRADY, RC ;
PETTIT, R .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1981, 103 (05) :1287-1289
[3]   ACTIVATION STUDIES WITH A PROMOTED PRECIPITATED IRON FISCHER-TROPSCH CATALYST [J].
BUKUR, DB ;
LANG, XS ;
ROSSIN, JA ;
ZIMMERMAN, WH ;
ROSYNEK, MP ;
YEH, EB ;
LI, CP .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1989, 28 (08) :1130-1140
[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]  
Dry M.E., 1981, The Fischer-Tropsch Synthesis, P159
[6]   Steady state isotopic transient kinetic analysis (SSITKA) of CO hydrogenation on different Co catalysts [J].
Froseth, V ;
Storsæter, S ;
Borg, O ;
Blekkan, EA ;
Ronning, M ;
Holmen, A .
APPLIED CATALYSIS A-GENERAL, 2005, 289 (01) :10-15
[7]  
GOODWIN JG, 2004, CATALYSIS, pCH8
[8]  
Hammache S., 2002, ENCY SURFACE COLLOID, V1, P2445
[9]   Effect of zirconia-modified alumina on the properties of Co/γ-Al2O3 catalysts [J].
Jongsomjit, B ;
Panpranot, J ;
Goodwin, JG .
JOURNAL OF CATALYSIS, 2003, 215 (01) :66-77
[10]   Impact of Cr, Mn and Zr addition on Fe Fischer-Tropsch synthesis catalysis: Investigation at the active site level using SSITKA [J].
Lohitharn, Nattaporn ;
Goodwin, James G., Jr. .
JOURNAL OF CATALYSIS, 2008, 257 (01) :142-151