One of the most harmful compounds are nitrogen oxides. Currently, the common industrial method of nitrogen oxides emission control is selective catalytic reduction with ammonia (NH3-SCR). Among all of the recognized measures, NH3-SCR is the most effective and reaches even up to 90% of NOx conversion. The presence of the catalyst provides the surface for the reaction to proceed and lowers the activation energy. The optimum temperature of the process is in the range of 150–450 °C and the majority of the commercial installations utilize vanadium oxide (V2O5) supported on titanium oxide (TiO2) in a form of anatase, wash coated on a honeycomb monolith or deposited on a plate-like structures. In order to improve the mechanical stability and chemical resistance, the system is usually promoted with tungsten oxide (WO3) or molybdenum oxide (MoO3). The efficiency of the commercial V2O5-WO3-TiO2 catalyst of NH3-SCR, can be gradually decreased with time of its utilization. Apart from the physical deactivation, such as high temperature sintering, attrition and loss of the active elements by volatilization, the system can suffer from chemical poisoning. All of the presented deactivating agents pass for the most severe poisons of V2O5-WO3-TiO2. In order to minimize the harmful influence of H2O, SO2, alkali metals, heavy metals and halogens, a number of methods has been developed. Some of them improve the resistance to poisons and some are focused on recovery of the catalytic system. Nevertheless, since the amount of highly contaminated fuels combusted in power plants and industry gradually increases, more effective poisoning-preventing and regeneration measures are still in high demand.
Natural zeolite of the heulandite-type framework was modified with iron and tested as a catalyst for the selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR) in the temperature range of 150–450 °C. The catalyst was prepared at a laboratory scale in a powder form and then the series of experiments of its shaping into tablets was conducted. Physicochemical studies of the catalyst (N2 sorption at −196 °C, FT-IR, XRD, UV-vis) were performed to determine the textural and structural properties and identify the surface functional groups, the crystalline structure of the catalysts and the form and aggregation of the active phase. The activity tests over the shaped catalyst were performed industry-reflecting conditions, using tail gases from the pilot nitric acid plant. The influence of a temperature, catalyst load, and the amount of reducing agent (ammonia) on the NOx reduction process were investigated. The results of catalytic tests that were performed on model gas mixture showed that non-modified clinoptilolite exhibited around 58% conversion of NO at 450 °C. The temperature window of the shaped catalyst shifted to a higher temperature range in comparison to the powder sample. The catalytic performance of the shaped Fe-clinoptilolite in the industry-reflecting conditions was satisfactory, especially at 450 °C. Additionally, it was observed that the ratio of N2O concentration downstream and upstream of the catalytic bed was below 1, which indicated that the catalyst exhibited activity in both DeNOx and DeN2O process.
The goal of the study was to modify activated carbon (AC) with nitrogen groups and ceria and to test the obtained materials in low temperature selective catalytic reduction of nitrogen oxides. For that purpose, the starting AC was oxidized with HNO3 of various concentrations, modified with urea and doped with 0.5 wt.% of Ce. It was observed that the increased concentration of acid influenced the catalytic activity, since textural and surface chemistry of activated carbon was changed. The most active sample was that modified with 14 M HNO3 and it reached 96% of NO conversion at 300 °C. Additionally, the addition of Ce improved the catalytic performance of modified AC, and NO was reduced according to oxidation–reduction mechanism, characteristic for supported metal oxides. Nevertheless, the samples promoted with Ce emitted significantly higher amount of CO2 comparing to the non-promoted ones.
The application of layered zeolites of MWW topology in environmental catalysis has attracted growing attention in recent years; however, only a few studies have explored their performance in selective catalytic reduction with ammonia (NH3-SCR). Thus, our work describes, for the first time, the one-pot synthesis of Fe-modified NH3-SCR catalysts supported on MCM-22, MCM-36, and ITQ-2. The calculated chemical composition of the materials was Si/Al of 30 and 5 wt.% of Fe. The reported results indicated a correlation between the arrangement of MWW layers and the form of iron in the zeolitic structure. We have observed that one-pot synthesis resulted in high dispersion of Fe3+ sites, which significantly enhanced low-temperature activity and prevented N2O generation during the reaction. All of the investigated samples exhibited almost 100% NO conversion at 250 °C. The most satisfactory activity was exhibited by Fe-modified MCM-36, since 50% of NO reduction was obtained at 150 °C for this catalyst. This effect can be explained by the abundance of isolated Fe3+ species, which are active in low-temperature NH3-SCR. Additionally, SiO2 pillars present in MCM-36 provided an additional surface for the deposition of the active phase.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.