A molecular mechanism for Fischer-Tropsch catalysis

被引:11
作者
Carter, MK [1 ]
机构
[1] Carter Technol, Los Gatos, CA 95031 USA
关键词
Fischer-Tropsch; linear backbone; catalysis; molecular mechanism; transition metal;
D O I
10.1016/S1381-1169(01)00080-2
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 catalysts Co(HCN)(2)-Fe(HCN)(2)-Co(HCN)(2) and [Fe(HCN)(2)](3) were designed, produced and proven for Fischer-Tropsch conversion of synthesis gas to liquid, and waxy aliphatic hydrocarbons, respectively. Hydrocarbons formed upon exposure of the catalysts to synthesis gas at room temperature and above. Hydrogen cyanide, released from the catalysts, was shown by direct MS measurements to be converted initially to nitriles. Thus, hydrogen cyanide became an in situ model compound illuminating a C-1 molecular insertion mechanism. This mechanism accounted for all products. FTIR and GC-MS measurements indicated the type and distribution of liquid hydrocarbons produced. Linear hydrocarbons formed from CO/H-2 while branched hydrocarbons formed from a mixture of acetylene plus CO/H-2 demonstrating the initial C-1 species associated with the catalyst, whether it was CO, HCN or one carbon of acetylene, acted as both tether and terminus in the step-wise chain growth mechanism. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:193 / 206
页数:14
相关论文
共 43 条
[1]  
ARMSTRONG RS, 1990, POLYHEDRON, V9, P282
[2]  
BALL JI, 1967, ACTA CRYSTALLOGR, V23, P239
[3]  
BELLAMY LJ, 1975, INFRARED SPECTA COMP, P27
[4]   INSITU DRIFTS STUDY OF ADSORBED SPECIES IN THE HYDROGENATION OF CARBON OXIDES [J].
BENITEZ, JJ ;
ALVERO, R ;
CARRIZOSA, I ;
ODRIOZOLA, JA .
CATALYSIS TODAY, 1991, 9 (1-2) :53-60
[5]   STRUCTURAL CHARACTERIZATION OF A 4-ELECTRON DONATING, DOUBLY-BRIDGING ISOCYANIDE IN MU-P-CH3C6H4NC)MN2(PH2PCH2PPH2)2(CO)4 [J].
BENNER, LS ;
OLMSTEAD, MM ;
BALCH, AL .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1978, 159 (03) :289-298
[6]  
BENSON SW, 1960, FDN CHEM KINETICS, P610
[7]   INCORPORATION OF SURFACE CARBON INTO HYDROCARBONS DURING FISCHER-TROPSCH SYNTHESIS - MECHANISTIC IMPLICATIONS [J].
BILOEN, P ;
HELLE, JN ;
SACHTLER, WMH .
JOURNAL OF CATALYSIS, 1979, 58 (01) :95-107
[8]   HYDROGEN-ASSISTED DISSOCIATION OF CO ON A CATALYST SURFACE [J].
BLYHOLDER, G ;
LAWLESS, M .
LANGMUIR, 1991, 7 (01) :140-141
[9]   REACTIONS OF DIAZOMETHANE ON TRANSITION-METAL SURFACES AND THEIR RELATIONSHIP TO THE MECHANISM OF THE FISCHER-TROPSCH REACTION [J].
BRADY, RC ;
PETTIT, R .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (19) :6181-6182
[10]  
BRADY RC, 1981, AM CHEM SOC, V103, P1289