1.Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering and Technology,Tianjin University,Tianjin,China;2.Collaborative Innovation Center of Chemical Science and Engineering,Tianjin,China;3.State Key Laboratory of Engines,Tianjin University,Tianjin,China
Abstract:
N2O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N2O formation over Pt/BaO/Al2O3 catalyst. Three types of catalysts, Pt/BaO/Al2O3, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al2O3 + Pd/Al2O3) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al2O3) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H2/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H2-TPR techniques. In addition, temperature programmed reactions of NO with H2/CO were conducted to obtain further information about N2O formation mechanism. Compared with Pt/BaO/Al2O3, (Pt/BaO/ Al2O3 + Pd/Al2O3) produced less N2O and more NH3 during NOx storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al2O3 + Al2O3). Temperature programmed reactions of NO with H2/CO results showed that Pd/Al2O3 component in (Pt/BaO/Al2O3 + Pd/Al2O3) played an important role in NO reduction to NH3, and the formed NH3 could reduce NOx to N2 leading to a decrease in N2O formation. Most of N2O formed over (Pt-Pd/BaO/Al2O3 + Al2O3) was originated from Pd/BaO/Al2O3 component. H2-TPR results indicated Pd-Ba interaction resulted in more difficultto- reduce PdOx species over Pd/BaO/Al2O3, which inhibits the NO dissociation and thus drives the selectivity to N2O in NO reduction.