Summary: | In this paper, mechanistic aspects involved in the formation of N2O over Pt-BaO/Al2O3 and Rh-BaO/Al2O3 model NOx Storage-Reduction (NSR) catalysts are discussed. The reactivity of both gas-phase NO and stored nitrates was investigated by using H2 and NH3 as reductants. It was found that N2O formation involves the presence of gas-phase NO, since no N2O is observed upon the reduction of nitrates stored over both Pt- and Rh-BaO/Al2O3 catalyst samples. In particular, N2O formation involves the coupling of undissociated NO molecules with N-adspecies formed upon NO dissociation onto reduced Platinum-Group-Metal (PGM) sites. Accordingly, N2O formation is observed at low temperatures, when PGM sites start to be reduced, and disappears at high temperatures where PGM sites are fully reduced and complete NO dissociation takes place. Besides, N2O formation is observed at lower temperatures with H2 than with NH3 in view of the higher reactivity of hydrogen in the reduction of the PGM sites and onto Pt-containing catalyst due to the higher reducibility of Pt vs. Rh.
|