Role of active oxygen and NOx species in N2O decomposition over Fe-ferrierite

[Display omitted] ► Fe-FER employed as catalysts for N2O decomposition and selective oxidations. ► Surface species in N2O decomposition over Fe-FER are time and temperature dependent. ► Below 220°C and up to 30min of interaction predominantly Fe–O species are formed. ► Above 280°C mainly Fe–NOx spec...

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Bibliographic Details
Published in:Journal of catalysis 2012-05, Vol.289, p.164-170
Main Authors: Sobalík, Zdeněk, Tabor, Edyta, Nováková, Jana, Sathu, Naveen K., Závěta, Karel
Format: Article
Language:English
Subjects:
Active oxygen
Catalysis
Chemistry
Exact sciences and technology
Fe–NOx species
General and physical chemistry
Ion-exchange
Iron ferrierite
Mössbauer spectroscopy
N2O decomposition
Surface physical chemistry
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
Zeolites: preparations and properties
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Summary:[Display omitted] ► Fe-FER employed as catalysts for N2O decomposition and selective oxidations. ► Surface species in N2O decomposition over Fe-FER are time and temperature dependent. ► Below 220°C and up to 30min of interaction predominantly Fe–O species are formed. ► Above 280°C mainly Fe–NOx species are observed even after short interaction. Direct evidence for the formation of surface Fe–NOx species over iron ferrierites during decomposition of N2O was found with a combination of temperature-programmed desorption of adsorbed surface species and infrared and Mössbauer spectroscopies. Surface NOx species were produced via the conversion of a transiently formed Fe(III)–O by exposing iron ferrierites (Si/Al=8.7, Fe/Al=0.07–0.1) to N2O. The transformation of Fe(III)–O into Fe–NOx was time- and temperature- dependent. Below 280°C, predominantly Fe(III)–O species were formed; these species are known to be highly active in oxidations at low temperatures. A transformation of Fe(III)–O into Fe–NOx species occurred when the reaction temperature was increased or when the reaction time was increased at low temperatures. This resulted in the disappearance of the oxidation activity of iron ferrierite. In contrast, the formation of Fe–NOx species enhanced the rate of N2O decomposition. Once formed, NOx species were stable during the subsequent N2O decomposition.
ISSN:0021-9517
1090-2694
DOI:10.1016/j.jcat.2012.02.007