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 NO_x 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 DeNO_x and DeN₂O process.

In this paper, the design of experiments and response surface methodology were proposed to study ammonia oxidation process. The following independent variables were selected: the reactor’s load, the temperature of reaction and the number of catalytic gauzes, whereas ammonia oxidation efficiency and N₂O concentration in nitrous gases were assumed as dependent variables (response). Based on the achieved results, statistically significant mathematical models were developed which describe the effect of independent variables on the analysed responses. In case of ammonia oxidation efficiency, its achieved value depends on the reactor’s load and the number of catalytic gauzes, whereas the temperature in the studied range (870–910 °C) has no effect on this dependent variable. The concentration of nitrous oxide in nitrous gases depends on all three parameters. The developed models were used for the multi-criteria optimization with the application of desirability function. Sets of parameters were achieved for which optimization assumptions were met: maximization of ammonia oxidation efficiency and minimization of the N₂O amount being formed in the reaction.

Different variants for abatement of N₂O emission from nitric acid plants with the use of catalysts developed at Łukasiewicz-INS were analyzed. Activity tests on a pilot scale confirmed the high activity of the studied catalysts. A two-stage catalytic abatement of N₂O emission in nitric acid plants was proposed: by high-temperature decomposition in the nitrous gases stream (HT-deN₂O) and low-temperature decomposition in the tail gas stream (LT-deN₂O). The selection of the optimal variant for abatement of N₂O emission depends on the individual characteristics of the nitric acid plant: ammonia oxidation parameters, construction of ammonia oxidation reactor and temperature of the tail gas upstream of the expansion turbine. It was shown that the combination of both deN₂O technologies, taking into account their technological constraints (dimensions of the catalyst bed), allows for a greater abatement of N₂O emission, than the use of only one technology. This solution may be economically advantageous regarding the high prices of CO₂ emission allowances.

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 NO_x 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 NO_x 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 NO_x reduction, especially in the high-temperature range, where the NO_x conversion rate exceeded 90%.

The tightening standards of nitrogen oxides emission from industrial plants encourage nitric acid producers to search for new efficient solutions to meet the stringent emission limits. Industrial practice and the patent literature show that the effectiveness of deNO_x (SCR) and deN₂O technology is affected not only by the type and shape of the catalyst, but also by the method of its installation in a heterogenous catalytic reactor. The article presents the background of the problem, related to the emission of nitrogen oxides from nitric acid plants, and describes the technology of the tail gases purified from NO_x and N₂O. It shows various aspects that should be considered in designing reactors for deNO_x and deN₂O processes in nitric acid plants. The advantages and disadvantages of different catalytic basket designs, their industrial application and the direction of their design development were also indicated.

The design of experiments (DoEs) with response surface methodology (RSM) were used to investigate the effect of operating parameters on the ammonia oxidation process. In this paper, the influence of reactor’s load and temperature of reaction as independent variables was investigated. The efficiency of NH₃ oxidation to NO and N₂O concentration in nitrous gases gas was identified as response variables. As a result of these studies, statistically significant models for two responses variables were developed.