A fast transient kinetic study of the effect of H2 on the selective catalytic reduction of NO x with octane using isotopically labelled 15NO

• Published in: Journal of catalysis 2007-02, Vol.246 (1), p.1
• Main Authors: Breen, J P, Burch, R, Hardacre, C, Hill, C J, Rioche, C
• Format: Article
• Language: English
• Subjects: Catalysis; Chemistry; Hydrogen; Kinetics; Phase transitions; Pressure
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2006.11.017

The H2-assisted hydrocarbon selective catalytic reduction (HC-SCR) of NOx was investigated using fast transient kinetic analysis coupled with isotopically labelled 15NO. This allowed monitoring of the evolution of products and reactants during switches of H2 in and out of the SCR reaction mix. The results obtained with a time resolution of less than 1 s showed that the effect on the reaction of the removal or addition of H2 was essentially instantaneous. This is consistent with the view that H2 has a direct chemical effect on the reaction mechanism rather than a secondary one through the formation of "active" Ag clusters. The effect of H2 partial pressure was investigated at 245 degrees C, it was found that increasing partial pressure of H2 resulted in increasing conversion of NO and octane. It was also found that the addition of H2 at 245 degrees C had different effects on the product distribution depending on its partial pressure. The change of the nitrogen balance over time during switches in and out of hydrogen showed that significant quantities of N-containing species were stored when hydrogen was introduced to the system. The positive nitrogen balance on removal of H2 from the gas phase showed that these stored species continued to react after removal of hydrogen to form N2. [PUBLICATION ABSTRACT]