Direct versus Hydrogen-Assisted CO Dissociation

被引：164

作者：

Shetty, Sharan ^{[1
]}

Jansen, Antonius P. J. ^{[1
]}

van Santen, Rutger A. ^{[1
]}

机构：

[1] Eindhoven Univ Technol, Inst Complex Mol Syst, NL-5600 MB Eindhoven, Netherlands

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2009年 / 131卷 / 36期

关键词：

RU(11(2)OVER-BAR1) SURFACE; TROPSCH; HYDROCARBONS; TRANSITION; ADSORPTION; CHEMISTRY; MECHANISM; CARBONYL; METALS; FLAT;

D O I：

10.1021/ja9044482

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The mechanism of CO dissociation is a fundamental issue in the technologically important Fischer-Tropsch (F-T) process that converts synthesis gas into liquid hydrocarbons. In the present study, we propose that on a corrugated Ru surface consisting of active sixfold (i.e., fourfold + twofold) sites, direct CO dissociation has a substantially lower barrier than the hydrogen-assisted paths (i.e., via HCO or COH intermediates). This proves that the F-T process on corrugated Ru surfaces and nanoparticles with active sixfold sites initiates through direct CO dissociation instead of hydrogenated intermediates.

引用

页码：12874 / +

页数：4

共 21 条

[1] Structure sensitivity of the methanation reaction:: H2-induced CO dissociation on nickel surfaces [J].

Andersson, M. P. ;

Abild-Pedersen, F. ;

Remediakis, I. N. ;

Bligaard, T. ;

Jones, G. ;

Engbwk, J. ;

Lytken, O. ;

Horch, S. ;

Nielsen, J. H. ;

Sehested, J. ;

Rostrup-Nielsen, J. R. ;

Norskov, J. K. ;

Chorkendorff, I. .

JOURNAL OF CATALYSIS, 2008, 255 (01) :6-19

[2] Origin of selectivity switch in Fischer-Tropsch synthesis over Ru and Rh from first-principles statistical mechanics studies [J].

Chen, Jia ;

Liu, Zhi-Pan .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (25) :7929-7937

[3] Carbon monoxide dissociation on planar and stepped Ru(0001) surfaces [J].

Ciobica, IM ;

van Santen, RA .

JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (16) :3808-3812

[4] Carbon monoxide dissociation on Rh nanopyramids [J].

de Mongeot, F. Buatier ;

Toma, A. ;

Molle, A. ;

Lizzit, S. ;

Petaccia, L. ;

Baraldi, A. .

PHYSICAL REVIEW LETTERS, 2006, 97 (05)

[5] CO dissociation on Ni: The effect of steps and of nickel carbonyl [J].

Engbaek, Jakob ;

Lytken, Ole ;

Nielsen, Jane H. ;

Chorkendorff, Lb .

SURFACE SCIENCE, 2008, 602 (03) :733-743

[6] CO adsorption on the multiple-site Ru(11(2)over-bar1) surface: The role of bonding competition [J].

Fan, CY ;

Bonzel, HP ;

Jacobi, K .

JOURNAL OF CHEMICAL PHYSICS, 2003, 118 (21) :9773-9782

[7]

Fischer F., 1923, BRENNST CHEM, V4, P276

[8] Adsorption and activation of CO over flat and stepped Co surfaces: A first principles analysis [J].

Ge, Qingfeng ;

Neurock, Matthew .

JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (31) :15368-15380

[9] CHx hydrogenation on Co(0001):: A density functional theory study -: art. no. 024711 [J].

Gong, XQ ;

Raval, R ;

Hu, P .

JOURNAL OF CHEMICAL PHYSICS, 2005, 122 (02)

[10] Fischer-tropsch mechanism revisited: Alternative pathways for the production of higher hydrocarbons from synthesis gas [J].

Inderwildi, Oliver R. ;

Jenkins, Stephen J. ;

King, David A. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (05) :1305-1307

← 1 2 3 →