Chain growth mechanism in Fischer-Tropsch synthesis: A DFT study of C-C coupling over Ru, Fe, Rh, and Re surfaces

被引：120

作者：

Cheng, Jun ^{[1
]}

Hu, P. ^{[1
]}

Ellis, Peter ^{[2
]}

French, Sam ^{[2
]}

Kelly, Gordon ^{[3
]}

Lok, C. Martin ^{[3
]}

机构：

[1] Queens Univ Belfast, Sch Chem, Belfast BT9 5AG, Antrim, North Ireland

[2] Johnson Matthey Technol Ctr, Reading RG4 9NH, Berks, England

[3] Johnson Matthey Technol Ctr, Billingham TS23 1LB, Cleveland, England

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2008年 / 112卷 / 15期

关键词：

D O I：

10.1021/jp711051e

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：

A quantitative approach is used to understand the chain growth mechanism in FT synthesis on the Ru, Fe, Rh, and Re surfaces. The C-C coupling reactions are extensively calculated on the stepped metal surfaces. Combining the coupling barriers and reactant stabilities, we investigate the reaction rates of all possible C, + C-1 coupling pathways on the metal surfaces. It is found that (i) all the transition-state structures are similar on these surfaces, while some coupling barriers are very different; (ii) the dominant chain growth pathways on these surfaces are different: C + CH and CH + CH on Rh and Ru surfaces, C + CH3 on Fe surface, and C + CH on Re surface. The common features of the major coupling reactions together with those on the Co surface are also discussed.

引用

页码：6082 / 6086

页数：5

共 53 条

[1] CO oxidation on Pt(111): An ab initio density functional theory study [J].

Alavi, A ;

Hu, PJ ;

Deutsch, T ;

Silvestrelli, PL ;

Hutter, J .

PHYSICAL REVIEW LETTERS, 1998, 80 (16) :3650-3653

[2] MECHANISM OF HYDROCARBON SYNTHESIS OVER FISCHER-TROPSCH CATALYSTS [J].

BILOEN, P ;

SACHTLER, WMH .

ADVANCES IN CATALYSIS, 1981, 30 :165-216

[3]

BOUDART M, 1984, KINETICS HETEREGENOU

[4] 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

[5] 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

[6]

CHENG J, UNPUB

[7] A quantitative determination of reaction mechanisms from density functional theory calculations: Fischer-Tropsch synthesis on flat and stepped cobalt surfaces [J].

Cheng, Jun ;

Gong, Xue-Qing ;

Hu, P. ;

Lok, C. Martin ;

Ellis, Peter ;

French, Sam .

JOURNAL OF CATALYSIS, 2008, 254 (02) :285-295

[8] A density functional theory study of the a-olefin selectivity in Fischer-Tropsch synthesis [J].

Cheng, Jun ;

Song, Tao ;

Hu, P. ;

Lok, C. Martin ;

Ellis, Peter ;

French, Sam .

JOURNAL OF CATALYSIS, 2008, 255 (01) :20-28

[9] A theoretical study of CHx chemisorption on the Ru(0001) surface [J].

Ciobîca, IM ;

Frechard, F ;

van Santen, RA ;

Kleyn, AW ;

Hafner, J .

CHEMICAL PHYSICS LETTERS, 1999, 311 (3-4) :185-192

[10] Mechanisms for chain growth in Fischer-Tropsch synthesis over Ru(0001) [J].

Ciobîca, IM ;

Kramer, GJ ;

Ge, Q ;

Neurock, M ;

van Santen, RA .

JOURNAL OF CATALYSIS, 2002, 212 (02) :136-144

← 1 2 3 4 5 6 →