The effect of pretreatment on the reactivity of Fe-ZSM-5 catalysts for N2O decomposition: Dehydroxylation vs. steaming

• Published in: Applied catalysis. B, Environmental Environmental, 2008-05, Vol.80 (3-4), p.226-236
• Main Authors: Roy, Pijus K., Prins, Roel, Pirngruber, Gerhard D.
• Format: Article
• Language: English
• Subjects: Autoreduction; Catalysis; Chemistry; Dealumination; Defects; Exact sciences and technology; General and physical chemistry; Ion-exchange; Iron zeolite; Isotope labeling; Step response; Surface physical chemistry; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; Zeolites: preparations and properties
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2007.10.015

The N2O decomposition activity of the Fe-ZSM-5 catalysts, prepared by chemical vapor deposition (CVD) and aqueous ion exchange (IE), was studied after steaming and high temperature treatment at 1218K (HT) and compared with the activity of the corresponding non-steamed catalysts after pretreatment at 873K. FTIR spectra showed that dehydroxylation and/or dealumination took place during steaming and high temperature treatment of the catalysts, which leads to the formation of oxygen vacancies (i.e. lattice defect). These lattice defects leads to a change in electronic properties of the iron sites, which are associated with electron withdrawing Al Lewis centers. The iron sites in close proximity of defects are responsible for the initial higher N2O decomposition (transient activity) of the steamed and HT catalysts. The increase in steady-state activity over steamed and HT catalysts can be mainly attributed to an increase in the number of active sites created by autoreduction of the iron centers during steaming and high temperature treatment. The above-mentioned trends are valid for both CVD and IE samples.