Dynamic Interplay between Diffusion and Reaction: Nitrogen Recombination on Rh{211} in Car Exhaust Catalysis
- 25 January 2008
- journal article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 130 (7), 2213-2220
- https://doi.org/10.1021/ja0754913
Abstract
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.Keywords
This publication has 34 references indexed in Scilit:
- An Unexpected Pathway for the Catalytic Oxidation of Methylidyne on Rh{111} as a Route to SyngasJournal of the American Chemical Society, 2007
- Influence of Coadsorbates on the NO Dissociation on a Rhodium(311) SurfaceChemphyschem, 2005
- Linear relationship between activation energies and reaction energies for coverage-dependent dissociation reactions on rhodium surfacesPhysical Chemistry Chemical Physics, 2005
- Structure and catalytic processes of N-containing species on Rh(111) from first principlesJournal of Catalysis, 2005
- Quantifying lateral adsorbate interactions by kinetic Monte-Carlo simulations and density-functional theory: NO dissociation on Rh(100)Physical Chemistry Chemical Physics, 2004
- A catalytic NOx reduction system using periodic steps, lean and rich operationsCatalysis Today, 2002
- Breaking the NO bond on Rh, Pd, and Pd3Mn alloy (100) surfaces: A quantum chemical comparison of reaction pathsThe Journal of Chemical Physics, 2001
- A catalytic NOx reduction system using periodic two steps: an operation in oxidizing conditions and a relatively short operation in reducing conditionsApplied Catalysis B: Environment and Energy, 2001
- Automotive Exhaust Emissions Control Using the Three-Way Catalyst System. 1. Computer Simulation of the NO-H2-O2 Reaction on Pt/AI2O3 CatalystIndustrial & Engineering Chemistry Product Research and Development, 1979
- Special points for Brillouin-zone integrationsPhysical Review B, 1976