Abstract
The adsorption of NO, NH3, H2O, and SO2 gaseous molecules on different transition metal oxides was studied based on density function theory (DFT), and three better-performing transition metal elements (Fe, Co, and Ce) were selected. Cu–Mn/SAPO-34 catalysts were prepared by impregnation method and then modified by the selected transition metals (Fe, Co, and Ce); the SO2 resistance experiments and characterizations including Brunner−Emmet−Teller (BET), X-ray Diffraction (XRD), Scanning Electronic Microscopy (SEM), and thermal gravity analysis (TG)-differential thermal gravity (DTG) before and after SO2 poisoning were conducted. The results showed that the deactivation of the Cu–Mn/SAPO-34 catalyst is ascribed to the deposition of lots of ammonium sulfates on the surface, depositing on the active sites and inhibiting the adsorption of NH3. After the modification of Fe, Co, and Ce oxides, the SO2 resistance of the modified Cu–Mn/SAPO-34 catalyst was significantly enhanced due to the less formation of ammonium sulfates. Among all these modified Cu–Mn/SAPO-34 catalysts, the Cu–Mn–Ce/SAPO-34 exhibited the highest SO2 resistance owing to the decreased decomposition temperature and the trapper of ceria for capturing SO2 to form Ce(SO4)2, further inhibiting the deposition of ammonium sulfates.
Highlights
Selective catalytic reduction with NH3 (NH3 -SCR) is considered as one of the most efficient techniques to control NOx emissions [1,2]
For the modified Cu–Mn/SAPO-34 catalyst by Fe, Co, and Ce oxides, the SO2 resistance performance is enhanced significantly owing to less deposition of ammonium sulfates, which can be observed intuitively by the Scanning Electronic Microscopy (SEM)-EDX analysis
The SCR activity of Cu–Mn/SAPO-34 catalyst modified by Fe, Co, and Ce oxides in the absence/presence were tested
Summary
Selective catalytic reduction with NH3 (NH3 -SCR) is considered as one of the most efficient techniques to control NOx emissions [1,2]. They concluded that the enhanced SCR performance is attributed to more generation of Oα species and promoted synergistic interaction among metal oxides by the doping of fluorine. Another method is to improve the preparation method of the Mn-based catalyst. Found that the MnO2 -based catalyst prepared by impregnation method in acetic acid solvent shows better SCR activity and SO2 resistance than in deionized water, anhydrous ethanol, and oxalic acid, owing to the evenly dispersed MnOx and enhanced interaction between metal oxides. It is expected that the present work will obtain more insights into improving the SO2 resistance to low-temperature SCR reaction over the Cu–Mn/SAPO-34 catalyst
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