Transient studies of direct N2O decomposition over Pt-Rh gauze catalyst. Mechanistic and kinetic aspects of oxygen formation

For elucidating the mechanistic aspects of oxygen formation during N2O decomposition over commercial woven Pt–Rh gauze, transient experiments were carried out in the temporal analysis of products (TAP) reactor by pulsing N216O over 18O-pretreated gauze catalyst at temperatures typical of industrial...

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Bibliographic Details
Published in:Catalysis letters 2003-12, Vol.91 (3-4), p.211-216
Main Authors: KONDRATENKO, Evgueni V, PEREZ-RAMIREZ, Javier
Format: Article
Language:English
Subjects:
Ammonia
Catalysis
Catalysts
Catalytic reactions
Chemistry
Decomposition
Exact sciences and technology
Gauze
General and physical chemistry
Nitrous oxide
Oxygen
Rhodium
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
Transient response
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Summary:For elucidating the mechanistic aspects of oxygen formation during N2O decomposition over commercial woven Pt–Rh gauze, transient experiments were carried out in the temporal analysis of products (TAP) reactor by pulsing N216O over 18O-pretreated gauze catalyst at temperatures typical of industrial ammonia burners (1073–1273 K). The transient responses of N2O and the products of its decomposition (O2 and N2) were fitted to two different mechanistic models. From the isotopic studies and the fitting of transient experiments, two separate routes of oxygen formation during catalytic N2O decomposition have been identified. Oxygen is produced via both (i) interaction of N2O with adsorbed oxygen species formed from N2O and (ii) recombination of adsorbed oxygen species on the catalyst surface. The relative contribution of these reaction pathways depends on the reaction temperature.
ISSN:1011-372X
1572-879X
DOI:10.1023/B:CATL.0000007157.87417.fe