Browsing by Subject "Selective catalytic reduction"
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Item Open Access Characterization of niobium-zirconium mixed oxide as a novel catalyst for selective catalytic reduction of NO x(2009) Cayirtepe, I.; Naydenov, A.; Ivanov, G.; Kantcheva, M.The performance of mixed niobium-zirconium oxide in the SCR of NO x with propene in excess oxygen has been studied. The mixed oxide is prepared by impregnation of hydrated zirconia with acidic solution (pH 0.5) of peroxoniobium(V) complex, [Nb2(O2)3] 4+, ensuring ZrO2:Nb2O5 mole ratio of 6:1. The calcined sample (denoted as 25NbZ-P) has the structure of Zr 6Nb2O17. According to the catalytic test, the conversion of NO x over the 25NbZ-P catalyst passes through a maximum at 220 °C. Based on the in situ FT-IR results, a reaction mechanism is proposed with nitroacetone and NCO species as the key reaction intermediates. The results of the investigation show that the catalytic properties of the Zr6Nb2O17 solid solution could be of interest regarding the development of low-temperature catalyst for the SCR of NO x with hydrocarbons. © 2009 Springer Science+Business Media, LLC.Item Open Access N-O activation on precious metal-free metal oxide based NOx removal systems(2022-01) Ercan, Kerem EmreElevated operational costs of platinum group metal (PGM) based environmental catalytic systems shift the focus of catalysis research towards cost-effective materials. In search for PGM-free alternative catalytic materials for NOx removal, high catalytic performance and long catalyst lifetime emerge as two important technical challenges. Within the scope of this dissertation, novel B-site mixed perovskites LaCoxMn1-xO3 (x = 0.1-0.9) and Fe and/or Co based CeO2 catalysts were synthesized, investigated and optimized as high performance, PGM-free, and durable catalyst alternatives for NOx removal systems. The perovskite based catalytic architectures can be utilized as diesel oxidation catalyst (DOC) oxidizing NO/CO to NO2/CO2, which can be coupled with selective catalytic reduction (SCR) catalysts to reduce NOx species to N2. On the other hand, Fe/Co based CeO2 systems can be exploited as catalyst candidates in SCR of NOx. In both of these NOx aftertreatment systems, NO activation is required. A simple and reproducible synthetic protocol was utilized to obtain perovskite-based DOC catalysts whose comprehensive structural characterization was carried out via XRD, N2 adsorption-desorption isotherm, ICP-MS, TEM, H2-TPR, ex-situ and in-situ XANES, EXAFS, in-situ FTIR, XPS, and TPD techniques. The oxidative catalytic performance of the perovskites for CO and NO oxidation was determined in flow-mode catalytic activity tests. It was demonstrated that bulk-oxygen vacancies have a strong influence on the redox activity of the B-site mixed perovskites with the ABO3 structure (where A = La, B = Co, Mn) allowing them to efficiently switch between high and low oxidation states in a reversible fashion under relatively moderate redox conditions without requiring elevated temperatures for regeneration, unlike conventional LaMnO3 and LaCoO3-based simple perovskite systems. La1.01Co0.75Mn0.24O2.97 and La1.04Co0.65Mn0.31O2.97 were found to reveal the best NO and CO oxidation performances among the currently investigated perovskites (La1.01Co0.75Mn0.24O2.97, La1.04Co0.65Mn0.31O2.97, La0.97Co1.03O2.91, and La0.97Mn1.03O3.17), which were on par with a conventional precious-metal benchmark catalyst (i.e., 1 wt. % Pt/Al2O3). Influence of Fe and Co loading on monometallic (Fe or Co) or bimetallic (Fe- Co) catalysts with different CeO2 support materials were studied in SCR of NO to N2. The flow-mode NO reduction experiments point out that 4 wt. % Co/CeO2 is the best catalyst in the studied group of catalysts based on its high N2 selectivity at relatively low temperatures. Detailed structural characterization experiments conducted via XRD, N2 adsorption-desorption isotherm, ATR-FTIR, Raman, and in-situ FTIR techniques indicate correlations between catalyst structure and SCR functionality. Our experimental findings indicate that 4 wt. % Co/CeO2 has relatively higher catalytic performance under excess H2(g) concentrations. The NO activation performance of both La1.01Co0.75Mn0.24O2.97 and La1.04Co0.65Mn0.31O2.97 B-site mixed perovskites and 4 wt. % Co/CeO2 were tested under significantly harsh conditions indicating their strong potential to be used not only in mobile applications but also in stationary NOx removal systems.