New insight into the in situ so2 poisoning mechanism over cu-ssz-13 for the selective catalytic reduction of nox with nh3

Abstract

To reveal the nature of SO2 poisoning over Cu-SSZ-13 catalyst under actual exhaust conditions, the catalyst was pretreated at 200 and 500◦ C in a flow containing NH3, NO, O2, SO2, and H2O. Brunner−Emmet−Teller (BET), X-ray diffraction(XRD), thermo gravimetric analyzer (TGA), ultraviolet Raman spectroscopy (UV Raman), temperature-programmed reduction with H2 (H2-TPR), temperature-programmed desorption of NO+O2 (NO+O2-TPD), NH3-TPD, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), and an activity test were utilized to monitor the changes of Cu-SSZ-13 before and after in situ SO2 poisoning. According to the characterization results, the types and generated amount of sulfated species were directly related to poisoning temperature. Three sulfate species, including (NH4 )2SO4, CuSO4, and Al2 (SO4 )3, were found to form on CZ-S-200, while only the latter two sulfate species were observed over CZ-S-500. Furthermore, SO2 poisoning had a negative effect on low-temperature selective catalytic reduction (SCR) activity, which was mainly due to the sulfation of active sites, including Z2 Cu, ZCuOH, and Si-O(H)-Al. In contrast, SO2 poisoning had a positive effect on high-temperature SCR activity, owing to the inhibition of the NH3 oxidation reaction. The above findings may be a useful guideline to design excellent SO2-resistant Cu-based zeolite catalysts.