A quantum-chemical DFT study of CO dissociation on Fe-promoted stepped Rh surfaces

被引：12

作者：

Filot, Ivo A. W. ^{[1
]}

Fariduddin, Farid ^{[1
]}

Broos, Robin J. P. ^{[1
]}

Zijlstra, Bart ^{[1
]}

Hensen, Emiel J. M. ^{[1
]}

机构：

[1] Eindhoven Univ Technol, Lab Inorgan Mat Chem, Schuit Inst Catalysis, Dept Chem Engn & Chem, POB 513, NL-5600 MB Eindhoven, Netherlands

来源：

CATALYSIS TODAY | 2016年 / 275卷

关键词：

Fischer-Tropsch; Rhodium; Iron; CO dissociation; DFT; ETHANOL SYNTHESIS; CATALYSTS; SYNGAS; CONVERSION; HYDROGENATION; TRANSITION; ENERGY; NANOPARTICLES; ALCOHOLS; METHANOL;

D O I：

10.1016/j.cattod.2015.10.009

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The present density functional theory study provides insight into the effect of Fe promotion on the CO dissociation reaction on a stepped Rh surface. On the basis of a density of states analysis we demonstrate that Fe is able to promote the CO dissociation reaction by stabilizing the oxygen atom in the transition state. This effect critically depends on the location of the Fe substitution in the Rh(211) surface and the pathway of the CO dissociation reaction. This work explains the higher activity and selectivity encountered in experimental studies during CO hydrogenation on Rh nanoparticles. (C) 2015 Elsevier B.V. All rights reserved.

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页码：111 / 118

页数：8

相关论文

共 46 条

[1] The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis [J].

Bligaard, T ;

Norskov, JK ;

Dahl, S ;

Matthiesen, J ;

Christensen, CH ;

Sehested, J .

JOURNAL OF CATALYSIS, 2004, 224 (01) :206-217

[2] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[3] MOLECULAR ORBITAL VIEW OF CHEMISORBED CARBON MONOXIDE [J].

BLYHOLDER, G .

JOURNAL OF PHYSICAL CHEMISTRY, 1964, 68 (10) :2772-&

[4] The preparation and characterisation of Fe-promoted Al2O3-supported Rh catalysts for the selective production of ethanol from syngas [J].

Burch, R ;

Hayes, MJ .

JOURNAL OF CATALYSIS, 1997, 165 (02) :249-261

[5] INVESTIGATION OF THE SYNTHESIS OF OXYGENATES FROM CARBON-MONOXIDE HYDROGEN MIXTURES ON SUPPORTED RHODIUM CATALYSTS [J].

BURCH, R ;

PETCH, MI .

APPLIED CATALYSIS A-GENERAL, 1992, 88 (01) :39-60

[6] THE EFFECT OF ALKALI PROMOTION ON CO HYDROGENATION OVER RH/TIO2 [J].

CHUANG, SC ;

GOODWIN, JG ;

WENDER, I .

JOURNAL OF CATALYSIS, 1985, 95 (02) :435-446

[7] Quantum chemistry of the Fischer-Tropsch reaction catalysed by a stepped ruthenium surface [J].

Filot, I. A. W. ;

van Santen, R. A. ;

Hensen, E. J. M. .

CATALYSIS SCIENCE & TECHNOLOGY, 2014, 4 (09) :3129-3140

[8] First-Principles-Based Microkinetics Simulations of Synthesis Gas Conversion on a Stepped Rhodium Surface [J].

Filot, Ivo A. W. ;

Broos, Robin J. P. ;

van Rijn, Jeaphianne P. M. ;

van Heugten, Gerardus J. H. A. ;

van Santen, Rutger A. ;

Hensen, Emiel J. M. .

ACS CATALYSIS, 2015, 5 (09) :5453-5467

[9] The Optimally Performing Fischer-Tropsch Catalyst [J].

Filot, Ivo A. W. ;

van Santen, Rutger A. ;

Hensen, Emiel J. M. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (47) :12746-12750

[10] Size and Topological Effects of Rhodium Surfaces, Clusters and Nanoparticles on the Dissociation of CO [J].

Filot, Ivo A. W. ;

Shetty, Sharan G. ;

Hensen, Emiel J. M. ;

van Santen, Rutger A. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (29) :14204-14212

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