Utilization of reducible mixed metal oxides as promoters for the enhancement of sulfur regeneration in nsr catalysts
Embargo Lift Date: 2017-01-01
Samast, Zehra Aybegüm
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Pt functionalized binary, ternary, and quaternary oxides (e.g. Pt/BaO/CeO2/ZrO2/Al2O3) were synthesized by wetness impregnation method and characterized by X-ray Diffraction (XRD), Brunauer–Emmett–Teller (BET) surface area analysis, in-situ Fourier Transform Infrared (FTIR), and temperature programmed desorption (TPD) techniques. Effect of the synthesis sequence on the NOx storage capacity was investigated by synthesizing subsequently impregnated and co-impregnated ternary oxides. Influence of BaO loading on NOx uptake of quaternary oxides was examined by utilizing two different BaO loadings namely; 8 wt% and 20 wt% on co-impregnated ternary oxide, Pt10-10CeZrAl. Co-presence of CeO2-ZrO2 oxide domains leads to an increase in NOx storage. As BaO loading increases in quaternary oxides, thermal stabilities of nitrates and nitrites increase due to the formation of bulk/ionic nitrates. Although BaO impregnation on co-impregnated ternary oxides leads to a decrease in specific surface area (SSA) values due to sintering, NOx adsorption on BaO-functionalized quaternary oxides was found to be higher than the BaO deficient ternary oxides. Upon sulfur poisoning, formation of strongly bound bulk/ionic sulfate/sulfite functional groups on BaO containing catalysts result in a need for higher temperatures for complete sulfur regeneration. Comparison of the CeO2-ZrO2 promoted systems with that of the Pt/ 20 wt% Ba/Al2O3 conventional NOx Storage Reduction (NSR) catalyst suggests that ceria-zirconia promotion enhances the sulfur tolerance. In conclusion, in this study a new NSR catalyst namely, Pt20Ba10-10CeZrAl, which is promoted with reducible mixed metal oxides, was synthesized and characterized. This novel NSR catalyst formulation revealed favorable sulfur resistance with minor sacrifice in NOx storage ability.