Adsorption and reaction of CO and hydrogen on iron-based Fischer-Tropsch synthesis catalysts

被引:95
作者
Zhang, Chenghua [1 ]
Zhao, Guoyan [1 ]
Liu, Kangkai [1 ]
Yang, Yong [1 ]
Xiang, Hongwei [1 ]
Li, Yongwang [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
基金
中国国家自然科学基金;
关键词
Fischer-Tropsch synthesis; Iron catalyst; H-2; adsorption; CO adsorption; Carbon hydrogenation; DENSITY-FUNCTIONAL THEORY; CARBON-MONOXIDE; SUPPORTED IRON; MOSSBAUER-SPECTROSCOPY; RAMAN-SPECTROSCOPY; SURFACE CARBON; CHEMISORPTION; POTASSIUM; H-2; TRANSITION;
D O I
10.1016/j.molcata.2010.05.020
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
H-2, CO chemisorptions and the carbon hydrogenation on promoted iron Fischer-Tropsch synthesis (FTS) catalysts (Fe/SiO2 and FeK/SiO2) were investigated using temperature programmed surface reaction with X-ray photoelectron spectroscopy and laser Raman spectroscopy. It is found that potassium, used as promoter, does not lead to a distinct variation in the carbon species but changes the surface H/C ratio of carburized catalysts. Besides bulk iron carbide, several carbon species with different cluster sizes exist in the carburized catalysts, which have different reactivities towards hydrogen. The surface atomic carbon, the oligomerized carbon species and the bulk iron carbide are more reactive to hydrogen, whereas the large-size amorphous carbons are relatively inert to hydrogen. There is a good correlation between the chemisorption of H-2 or CO and the corresponding feed gas conversion activity in FTS reaction. Meanwhile, the methane selectivity is correlated with the hydrogenation capability of catalysts, indicating that the surface H concentration has an important effect on the selectivity of hydrocarbons. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:35 / 43
页数:9
相关论文
共 48 条
[1]   CHEMISORPTION OF GASES ON A PROMOTED IRON CATALYST .1. HYDROGEN, NITROGEN, CARBON-MONOXIDE AND CARBON-DIOXIDE [J].
AMENOMIYA, Y ;
PLEIZIER, G .
JOURNAL OF CATALYSIS, 1973, 28 (03) :442-454
[2]   Methane dissociation and syngas formation on Ru, Os, Rh, Ir, Pd, Pt, Cu, Ag, and Au: A theoretical study [J].
Au, CT ;
Ng, CF ;
Liao, MS .
JOURNAL OF CATALYSIS, 1999, 185 (01) :12-22
[3]  
BARO AM, 1981, SURF SCI, V112, pL759, DOI 10.1016/0039-6028(81)90324-1
[4]   THE EFFECTS OF CARBON, OXYGEN, SULFUR AND POTASSIUM ADLAYERS ON CO AND H-2 ADSORPTION ON FE(100) [J].
BENZIGER, J ;
MADIX, RJ .
SURFACE SCIENCE, 1980, 94 (01) :119-153
[5]   NATURE OF SURFACE SPECIES ON SUPPORTED IRON DURING CO/H2 REACTION [J].
BIANCHI, D ;
TAU, LM ;
BORCAR, S ;
BENNETT, CO .
JOURNAL OF CATALYSIS, 1983, 84 (02) :358-374
[6]   Study of the oxide/carbide transition on iron surfaces during catalytic coke formation [J].
Bonnet, F ;
Ropital, F ;
Lecour, P ;
Espinat, D ;
Huiban, Y ;
Gengembre, L ;
Berthier, Y ;
Marcus, P .
SURFACE AND INTERFACE ANALYSIS, 2002, 34 (01) :418-422
[7]   CHEMICAL NATURE OF THE CARBONACEOUS DEPOSITS ON IRON AFTER CO HYDROGENATION [J].
BONZEL, HP ;
KREBS, HJ .
SURFACE SCIENCE, 1980, 91 (2-3) :499-513
[8]   CHEMISORPTION OF HYDROGEN ON IRON SURFACES [J].
BOZSO, F ;
ERTL, G ;
GRUNZE, M ;
WEISS, M .
APPLICATIONS OF SURFACE SCIENCE, 1977, 1 (01) :103-119
[9]   LONG-RANGE POISONING OF D2 DISSOCIATIVE CHEMISORPTION ON PT(111) BY COADSORBED-K [J].
BROWN, JK ;
LUNTZ, AC ;
SCHULTZ, PA .
JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (05) :3767-3774
[10]   CHEMISORPTION AND REACTION OF ACETYLENE AND ETHYLENE ON ALPHA-FE(100) CLEAN IRON SURFACE [J].
BRUCKER, C ;
RHODIN, T .
JOURNAL OF CATALYSIS, 1977, 47 (02) :214-231