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.
In modern dual-pressure nitric acid plants, the tail gas temperature usually exceeds 300 °C. The NH3-SCR catalyst used in this temperature range must be resistant to thermal deactivation, so commercial vanadium-based systems, such as V2O5-WO3 (MoO3)-TiO2, are most commonly used. However, selectivity of this material significantly decreases above 350 °C due to the increase in the rate of side reactions, such as oxidation of ammonia to NO and formation of N2O. Moreover, vanadium compounds are toxic for the environment. Thus, management of the used catalyst is complicated. One of the alternatives to commercial V2O5-TiO2 catalysts are natural zeolites. These materials are abundant in the environment and are thus relatively cheap and easily accessible. Therefore, the aim of the study was to design a novel iron-modified zeolite catalyst for the reduction of NOx emission from dual-pressure nitric acid plants via NH3-SCR. The aim of the study was to determine the influence of iron loading in the natural zeolite-supported catalyst on its catalytic performance in NOx conversion. The investigated support was firstly formed into pellets and then impregnated with various contents of Fe precursor. Physicochemical characteristics of the catalyst were determined by XRF, XRD, low-temperature N2 sorption, FT-IR, and UV–Vis. The catalytic performance of the catalyst formed into pellets was tested on a laboratory scale within the range of 250–450 °C using tail gases from a pilot nitric acid plant. The results of this study indicated that the presence of various iron species, including natural isolated Fe3+ and the introduced FexOy oligomers, contributed to efficient NOx reduction, especially in the high-temperature range, where the NOx conversion rate exceeded 90%.