Modified Zeolite Catalyst for a NOx Selective Catalytic Reduction Process in Nitric Acid Plants

Abstract

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.