Reduction of nitrogen oxides by carbon monoxide over an iron oxide catalyst under dynamic conditions

The reduction of NO and N₂O by CO over a silica-supported iron oxide catalyst was investigated by the transient response method, with different initial oxidation states of the catalyst, i.e. completely reduced (Fe₃O₄), or oxidised (Fe₂O₃). The influence of CO pre-adsorption was also studied. From the material balance on the gas phase species, it was shown that the composition of the catalyst changes during relaxation to steady-state. The degree of reduction of the catalyst at steady-state could thus be estimated. During the transient period, CO was shown to inhibit N₂O as well as NO reductions by adsorption on reduced sites. The activity of the reduced catalyst was found to be substantially higher as compared to the oxidised catalyst for both reactions. On this basis, it was attempted to keep the catalyst in a reduced state by periodically reducing it with CO. As a result, a significant increase in the performance of the reactor with respect to steady-state operation could be achieved for N₂O reduction by CO. Finally, the dynamic behaviour of the N₂O–CO and NO–CO reactions made it possible to evidence reaction steps, the occurrence of which could not be shown during our previous investigations on the separate interactions of the reactants with the catalyst.