In Situ Scanning Tunneling Microscopy of the Dissociation of CO on Co(0001)

被引：40

作者：

Boeller, B. ^{[1
]}

Ehrensperger, M. ^{[1
]}

Wintterlin, J. ^{[1
,2
]}

机构：

[1] Univ Munich, Dept Chem, D-81377 Munich, Germany

[2] Ctr NanoSci, D-80799 Munich, Germany

来源：

ACS CATALYSIS | 2015年 / 5卷 / 11期

关键词：

Fischer-Tropsch; carbon monoxide; dissociation; Co(0001); in situ STM; XPS; SINGLE-CRYSTAL SURFACE; CARBON-MONOXIDE; COBALT CATALYSTS; TROPSCH; PRESSURE; CHEMISORPTION; ADSORPTION; ACTIVATION; REACTIVITY; MECHANISM;

D O I：

10.1021/acscatal.5b01684

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 dissociation of CO, a crucial step in the cobalt-catalyzed Fischer-Tropsch synthesis, was investigated by in situ scanning tunneling microscopy on Co(0001) at CO pressures up to 0.25 mbar and temperatures up to 493 K. A new type of surface reconstruction was observed that is formed by carbidic carbon, as shown by X-ray photoelectron spectroscopy. Using (CO)-C-13 and titrating C-13 with O-2, the surface carbon is shown to originate from CO. The results are in contrast to predictions by theoretical work. However, the dissociation rates are 3 orders of magnitude lower than the previously measured methanation rates under equivalent conditions.

引用

收藏

页码：6802 / 6806

页数：5

相关论文

共 33 条

[1] Origin of the Formation of Nanoislands on Cobalt Catalysts during Fischer-Tropsch Synthesis [J].

Banerjee, Arghya ;

van Bave, Alexander P. ;

Kuipers, Herman P. C. E. ;

Saeys, Mark .

ACS CATALYSIS, 2015, 5 (08) :4756-4760

[2]

Bartholomew CH, 2006, FUNDAMENTALS OF INDUSTRIAL CATALYTIC PROCESSES, 2ND EDITION, P339

[3] Polarization modulation infrared reflection absorption spectroscopy of CO adsorption on Co(0001) under a high-pressure regime [J].

Beitel, GA ;

Laskov, A ;

Oosterbeek, H ;

Kuipers, EW .

JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (30) :12494-12502

[4] A combined in-situ PM-RAIRS and kinetic study of single-crystal cobalt catalysts under synthesis gas at pressures up to 300 mbar [J].

Beitel, GA ;

deGroot, CPM ;

Oosterbeek, H ;

Wilson, JH .

JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (20) :4035-4043

[5] OXYGEN-CHEMISORPTION, SURFACE OXIDATION, AND THE OXIDATION OF CARBON-MONOXIDE ON COBALT(0001) [J].

BRIDGE, ME ;

LAMBERT, RM .

SURFACE SCIENCE, 1979, 82 (02) :413-424

[6] CHEMISORPTION STUDIES ON COBALT SINGLE-CRYSTAL SURFACES .1. CARBON-MONOXIDE ON CO(0001) [J].

BRIDGE, ME ;

COMRIE, CM ;

LAMBERT, RM .

SURFACE SCIENCE, 1977, 67 (02) :393-404

[7] ELECTRONIC-STRUCTURE CALCULATIONS AND DYNAMICS OF METHANE ACTIVATION ON NICKEL AND COBALT [J].

BURGHGRAEF, H ;

JANSEN, APJ ;

VANSANTEN, RA .

JOURNAL OF CHEMICAL PHYSICS, 1994, 101 (12) :11012-11020

[8] Adsorbate induced reconstruction of cobalt surfaces [J].

Ciobica, I. M. ;

van Santen, R. A. ;

van Berge, P. J. ;

de Loosdrecht, J. van .

SURFACE SCIENCE, 2008, 602 (01) :17-27

[9] C-H Bond Activation of Light Alkanes on Pt(111): Dissociative Sticking Coefficients, Evans-Polanyi Relation, and Gas-Surface Energy Transfer [J].

Cushing, G. W. ;

Navin, J. K. ;

Donald, S. B. ;

Valadez, L. ;

Johanek, V. ;

Harrison, I. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (40) :17222-17232

[10] On the Origin of the Cobalt Particle Size Effects in Fischer-Tropsch Catalysis [J].

den Breejen, J. P. ;

Radstake, P. B. ;

Bezemer, G. L. ;

Bitter, J. H. ;

Froseth, V. ;

Holmen, A. ;

de Jong, K. P. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (20) :7197-7203

← 1 2 3 4 →