Dynamic interplay between diffusion and reaction: Nitrogen recombination on Rh{211} in car exhaust catalysis

被引：21

作者：

Inderwildi, Oliver R. ^{[1
]}

Jenkins, Stephen J. ^{[1
]}

King, David A. ^{[1
]}

机构：

[1] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2008年 / 130卷 / 07期

基金：

英国工程与自然科学研究理事会;

关键词：

D O I：

10.1021/ja0754913

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The adsorption and diffusion of atomic nitrogen on Rh{211} as well as formation and desorption of molecular nitrogen from this surface have been investigated by means of density functional theory (DFT) calculations. The elementary step reaction mechanism derived from this comprehensive DFT study forms the foundation of a detailed microkinetic model including diffusion, recombination, and desorption of nitrogen species. It will be shown that nitrogen formation on a stepped rhodium surface is a dynamic interplay of atomic nitrogen diffusion and reaction. Moreover, evidence will be presented that not one but several on-step recombination reactions are responsible for dinitrogen formation and desorption.

引用

页码：2213 / 2220

页数：8

共 46 条

[31] A catalytic NO reduction in periodic lean and rich excursions over Rh supported on oxygen storage capacity materials [J].

Nakatsuji, T ;

Ruotoistenmäki, J ;

Komppa, V ;

Tanaka, Y ;

Uekusa, T .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2002, 38 (02) :101-116

[32] A catalytic NOx reduction system using periodic two steps:: an operation in oxidizing conditions and a relatively short operation in reducing conditions [J].

Nakatsuji, T ;

Komppa, V .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 30 (1-2) :209-223

[33] ATOMS, MOLECULES, SOLIDS, AND SURFACES - APPLICATIONS OF THE GENERALIZED GRADIENT APPROXIMATION FOR EXCHANGE AND CORRELATION [J].

PERDEW, JP ;

CHEVARY, JA ;

VOSKO, SH ;

JACKSON, KA ;

PEDERSON, MR ;

SINGH, DJ ;

FIOLHAIS, C .

PHYSICAL REVIEW B, 1992, 46 (11) :6671-6687

[34] Adsorption, diffusion, and dissociation of molecular oxygen at defected TiO2(110):: A density functional theory study [J].

Rasmussen, MD ;

Molina, LM ;

Hammer, B .

JOURNAL OF CHEMICAL PHYSICS, 2004, 120 (02) :988-997

[35] Density-functional theory calculations of hopping rates of surface diffusion [J].

Ratsch, C ;

Scheffler, M .

PHYSICAL REVIEW B, 1998, 58 (19) :13163-13166

[36] Structure and catalytic processes of N-containing species on Rh(111) from first principles [J].

Ricart, JM ;

Ample, F ;

Clotet, A ;

Curulla, D ;

Niemantsverdriet, JW ;

Paul, JF ;

Pérez-Ramírez, J .

JOURNAL OF CATALYSIS, 2005, 232 (01) :179-185

[37] Experimental and numerical study on the transient behavior of partial oxidation of methane in a catalytic, monolith [J].

Schwiedernoch, R ;

Tischer, S ;

Correa, C ;

Deutschmann, O .

CHEMICAL ENGINEERING SCIENCE, 2003, 58 (3-6) :633-642

[38] First-principles simulation: ideas, illustrations and the CASTEP code [J].

Segall, MD ;

Lindan, PJD ;

Probert, MJ ;

Pickard, CJ ;

Hasnip, PJ ;

Clark, SJ ;

Payne, MC .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2002, 14 (11) :2717-2744

[39] Flame-derived Pt/Ba/CexZr1-xO2:: Influence of support on thermal deterioration and behavior as NOx storage-reduction catalysts [J].

Strobel, Reto ;

Krumeich, Frank ;

Pratsinis, Sotiris E. ;

Baiker, Alfons .

JOURNAL OF CATALYSIS, 2006, 243 (02) :229-238

[40] Direct measurement of surface diffusion using atom-tracking scanning tunneling microscopy [J].

Swartzentruber, BS .

PHYSICAL REVIEW LETTERS, 1996, 76 (03) :459-462

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