Study on Novel SCR Catalysts for Denitration of High Concentrated Nitrogen Oxides and Their Reaction Mechanisms

Abstract

With the rapid development of industrialization, the emission of nitrogen oxides (NOx) has become a global environmental issue. Uranium is the primary fuel used in nuclear power generation. However, the production of uranium, typically based on the uranyl nitrate method, usually generates large amounts of nitrogen oxides, particularly NO2, with concentrations in the exhaust gas exceeding 10,000 ppm. High concentrations of nitrogen dioxide are also produced during silver electrolysis processing and the treatment of waste electrolyte solutions. Traditional V-W/TiO2 NH3-SCR catalysts typically exhibit high catalytic activity at temperatures ranging from 300 to 400 °C, under conditions of low NOx concentrations and high gas hourly space velocity. However, their performance is not satisfying when reducing high concentrations of NO2. This study aims to optimize the traditional V-W/TiO2 catalysts to enhance their catalytic activity under conditions of high NO2 concentrations (10,000 ppm) and a wide temperature range (200–400 °C). On the basis of 3 wt% Mo/TiO2, various loadings of V2O5 were selected, and their catalytic activities were tested. Subsequently, the optimal ratios of active component vanadium and additive molybdenum were explored. Simultaneously, doping with WO3 for modification was selected in the V-Mo/TiO2 catalyst, followed by activity testing under the same conditions. The results show that: the NOx conversion rates of all five catalysts increase with temperature at range of 200–400 °C. Excessive loading of MoO3 decreased the catalytic performance, with 5 wt% being the optimal loading. The addition of WO3 significantly enhanced the low-temperature activity of the catalysts. When the loadings of WO3 and MoO3 were both 3 wt%, the catalyst exhibited the best denitrification performance, achieving a NOx conversion rate of 98.8% at 250 °C. This catalyst demonstrates excellent catalytic activity in reducing very high concentration (10,000 ppm) NO2, at a wider temperature range, expanding the temperature range by 50% compared to conventional SCR catalysts. Characterization techniques including BET, XRD, XPS, H2-TPR, and NH3-TPD were employed to further study the evolution of the catalyst, and the promotional mechanisms are explored. The results revealed that the proportion of chemisorbed oxygen (Oα) increased in the WO3-modified catalyst, exhibiting lower V reduction temperatures, which are favorable for low-temperature denitrification activity. NH3-TPD experiments showed that compared to MoOx species, surface WOx species could provide more acidic sites, resulting in stronger surface acidity of the catalyst.