Content Summary | In the present study the technique of the in situ diffuse reflectance infrared Fourier
transform spectroscopy (DRIFTS) is used in order to explore the effect of electropositive
promoters, such as sodium, on the surface chemistry and catalytic behavior of Pt/γ-Al2O3
catalysts during the NO reduction by C3H6. It was found that under steady-state reaction
conditions the surface of un-promoted catalysts is mainly covered by carbon containing species
(hydrocarbon fragments, formates, acetates, cyanides), whereas that of Na-promoted catalysts is
predominantly covered by NOx ad-species, carbonyls and isocyanates, implying the significant
effect of Na promoter on the nature of adsorbed species. To further elucidate the role of Napromoter
on the nature and the reactivity of adsorbed species, the transient response of IR
spectra under the cycle: NO→He→C3H6→NO, is also investigated over both un-promoted and
Na-promoted catalysts. The results indicate that interaction of propene with NOx pre-adsorbed
species (mainly nitrates) over un-promoted Pt/Al2O3 catalysts results in the formation of strongly
bonded carboxylates and cyanide species, which are inactive towards NO. On the opposite, NO
adsorption over Na-promoted catalysts favours the formation of nitro/nitrite and nitrosyl species,
which are highly active towards propene, leading to the formation of enolic species (R-CH=CO),
organic compounds (CxHyNOz), isocyanates (NCO) and carbonyl (CO) species. Among these
species isocyanates are very active towards NO, leading to the formation of the gas phase
reaction products (i.e., N2, N2O, CO2, H2O). The present results demonstrate that the excellent
catalytic performance of sodium modified Pt/Al2O3 catalysts during the NO reduction by
propene, can be interpreted based on the significant modifications induced by the electropositive
promoter on the catalyst’s surface chemistry | en |