Li Cao,Xiaodong Wu,Ze Chen,Yue Ma,Ziran Ma,Rui Ran,Zhichun Si,Duan Weng,Baodong Wang
CeO 2 /WO 3 -TiO 2 (CeWTi) and Nb 2 O 5 -CeO 2 /WO 3 -TiO 2 (NbCeWTi) catalysts were prepared by a sol-gel precipitation method. Both the catalysts exhibit high selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) activities at 270–500 °C. The sulfur tolerances of the catalysts were evaluated at 270 °C by adding H 2 O and SO 2 in the feeding gas and NbCeWTi exhibited a significantly improved resistance. The thermogravimetric (TG) and mass spectrographic (MS) results indicated that much less sulfates formed on NbCeWTi and existed mainly in the form of ammonium hydrogen sulfate species which protected Ce x+ active sites effectively from attacking of SO 2 . According to the results of temperature-programmed desorption of ammonia (NH 3 -TPD), H 2 temperature-programmed reduction (H 2 -TPR) and SO 2 oxidation , loading niobia on CeWTi inhibited the SO 2 oxidative adsorption and SO 3 production which basically reduced sulfur poisoning of the catalyst. Additionally, the niobia modification ensured the formation of nitrates from the competitive adsorption of SO 2 and hereby facilitated the nitrate SCR route based on the in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS).
Two Ce-W-Ti mixed oxide catalysts were prepared by wet impregnation (CeW/Ti-I) and mechanical mixing (Ce/W/Ti-M) methods. CeW/Ti-I catalyst exhibits over 80% NO x conversion and nearly 100% N 2 selectivity at 200–550 °C. The superior catalytic performance is associated with the high dispersion of active CeO 2 and acidic WO 3 on TiO 2 and the synergistic effects among different components. The X-ray Diffraction, Raman spectroscopy, Nitrogen physisorption, X-ray photoelectron spectroscopy, H 2 temperature-programmed reduction, temperature-programmed desorption of ammonia and infrared spectroscopy were performed. It is found that the formation of solid solutions, as well as the high specific surface area, would increase the amounts of Ce 3+ , oxygen vacancies and acid sites in the catalyst. These broaden the operating temperature window of NH 3 -SCR reaction and enhance the N 2 selectivity by facilitating “fast SCR” reaction at low temperatures and inhibiting the unselective oxidation of NH 3 at high temperatures.
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