title: New Insights into the N2O formation mechanism over Pt-BaO/Al2O3 model catalysts using H2 as a reductant.
abstract: The N2O formation mechanism was investigated over a Pt-BaO/Al2O3 catalyst applied on light-duty diesel vehicles using H2 as a reductant in the absence and presence of H2O. In the absence of H2O, N2O forms mainly at the initial phase of lean NOx trapping; while in the presence of H2O, N2O appears mainly at the beginning of the rich reduction phase. In the lean period, N2O is formed via the gaseous NO/O2 reacting with the adsorbed H and NH3 that are formed during the previous rich period. The N2O formation in the rich period is insignificant in the absence of H2O but is greatly enhanced by the presence of H2O. The amount of N2O formed is proportional to the H2O level in the feed, and its formation is favored at low temperatures. Our FTIR data show that H2O enhances the rate of nitrite/nitrate reduction during the rich regeneration, which increases the amount of released NOx, an oxygen source for N2O formation. Our temperature-programmed experiments indicate that H2O competes with NH3 for adsorption sites on Pt surface. This competitive adsorption may increase the NH3 desorption rate at low temperatures in the rich phase and make Pt surface more accessible to NO.
authors.affiliation: Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering & Technology, Tianjin University , Tianjin 300072, PR China.
authors.forename: Jinxin
authors.initials: J
authors.lastname: Zhu
authors.forename: Jun
authors.initials: J
authors.lastname: Wang
authors.forename: Jianqiang
authors.initials: J
authors.lastname: Wang
authors.forename: Liangfang
authors.initials: L
authors.lastname: Lv
authors.forename: Xiuting
authors.initials: X
authors.lastname: Wang
authors.forename: Meiqing
authors.initials: M
authors.lastname: Shen
mesh_terms: D000327:Adsorption; D000537:Aluminum Oxide / Q000737:chemistry*; D017609:Barium Compounds / Q000737:chemistry*; D002384:Catalysis; D003080:Cold Temperature; D006859:Hydrogen / Q000737:chemistry*; D007700:Kinetics; D009609:Nitrous Oxide / Q000138:chemical synthesis*; D010087:Oxides / Q000737:chemistry*; D010984:Platinum / Q000737:chemistry*; D019163:Reducing Agents; D013696:Temperature
chemical_list: D017609:Barium Compounds; D010087:Oxides; D019163:Reducing Agents; D010984:Platinum; C077606:barium oxide; D006859:Hydrogen; D009609:Nitrous Oxide; D000537:Aluminum Oxide