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Partial Reduction of NO to N2O on Cu{311}: Role of Intermediate N2O2

Published version
Peer-reviewed

Type

Article

Change log

Authors

Temprano Farina, Israel 
Sitathani, Krit 
Jenkins, Stephen 

Abstract

We investigate the adsorption and reaction of NO on Cu{311} via a combination of Reflection Absorption Infrared Spectroscopy (RAIRS) and first-principles Density Functional Theory (DFT), providing a mechanistic understanding of the reaction as it progresses. Our results support an interpretation that N2O is formed via an associative mechanism involving N2O2 as the crucial intermediate species. Consistent with previous work, we find that such an intermediate readily converts between its initial nitrogen-down configuration and an inverted oxygen-down configuration, prior to decomposition by cleavage of a single N-O bond. As the reaction proceeds, the surface is progressively poisoned by the accumulation of O adatoms resulting from N-O bond scission, and we probe this aspect of the reaction in detail as a function both of temperature and of the surface’s pre-exposure to oxygen. Our results indicate that sustained conversion of NO to N2O on Cu would be contingent upon identifying some co-reactant capable of continuously removing O from the surface as the reaction proceeds

Description

Keywords

34 Chemical Sciences, 3406 Physical Chemistry

Journal Title

Catalysis Science & Technology

Conference Name

Journal ISSN

2044-4761
2044-4761

Volume Title

Publisher

Royal Society of Chemistry