Remarkable effect of addition of In and Pb on the reduction of N2O by CO over SiO2 supported Pd catalysts

The effect of addition of In and Pb on the reduction of N₂O by CO was studied over SiO₂ supported Pd catalysts, using a closed gas circulation system as well as in-situ infrared spectroscopy. Formation of intermetallic compounds such as Pd_0.48In_0.52, Pd₃Pb and Pd₃Pb₂ was observed which caused a drastic enhancement of the rate of N₂ formation. The infrared spectroscopic analyses revealed a weakening of the adsorption strength of CO on Pd metal by the formation of intermetallic compounds, which is likely the main reason for the enhancement of the reaction rate. From a kinetic investigation as well as in situ FT-IR observation during the N₂O-CO reaction, a redox mechanism was proposed involving the oxidation of the surface by N₂O followed by its reduction by CO. Over Pd/SiO₂, the former process seems to be the rate limiting step because of the inhibition of N₂O activation by strongly adsorbed CO. By adding In or Pb, the rate limiting step shifted to the latter process, which resulted in a large enhancement in the rate of N₂ formation.