A study on the selective catalytic reduction of NOx by ammonia on sulphated iron-based catalysts

Abstract

A series of sulphated iron-based catalysts was prepared via an impregnation method by changing the loading content of Fe³⁺ and SO₄²⁻ on ZrO₂, and their performance in the selective catalytic reduction (SCR) of NO_x by ammonia was investigated. The NO_x conversion exhibited large differences among the sulphated iron-based catalysts. To explore the synergistic mechanism of iron and sulphates, XRD, BET, H₂-TPR, XPS, TPD and in situ DRIFTS were used to characterize the catalysts, and it was found that among all the catalysts, the NO_x conversion by Fe₂SZr was greater than 90% at 350–450 °C. The results indicated that the interaction between Fe³⁺ and SO₄²⁻ can have an effect on the redox ability, acid sites, and adsorption of NO_x and NH₃. With an increase in the content of Fe³⁺, the redox activity of the catalyst and the adsorption of ammonia improved at medium and low temperatures. However, at higher temperatures, an increase in Fe³⁺ led to a decrease in the conversion of NO_x due to the enhanced oxidation of NH₃. At medium and low temperatures, an increase in the content of SO₄²⁻ decreased the concentration of Fe³⁺ on the surface of the catalyst and inhibited the adsorption of NO_x and NH₃. The addition of SO₄²⁻ reduced the redox activity of the catalyst and inhibited the oxidation reaction of NH₃, which follows the Eley–Rideal mechanism at high temperatures, further enhancing the SCR activity of the Fe_xS_yZr catalyst.