Selective catalytic reduction of NOx with NH3 over zeolite H–ZSM-5: influence of transient ammonia supply

The effect of ammonia supply on the selective catalytic reduction of NOx over zeolite H–ZSM-5 was investigated using step response experiments between 200 and 500 °C. For inlet NO:NO2 ratios > 1, the activity for NOx reduction transiently increased when NH3 was removed from the feed. For NO:NO2 ratios ⩽ 1, the NOx reduction however decreased. By pulsing NH3 to the feed, the activity for NO reduction was enhanced up to five times compared to continuous supply of ammonia. For NO:NO2 ratios exceeding one, also the selectivity towards N2O formation was lower with transient ammonia supply. Temperature programmed reaction experiments with preadsorbed NH3 showed highest initial NOx reduction activity when ammonia had been adsorbed at 300 or 250 °C compared to 200 °C. A minimum in NO reduction was observed at 130 °C independent of the ammonia adsorption temperature. For NO:NO2 ratios > 1, the results strongly indicate that NO oxidation is the rate determining step in the ammonia selective catalytic reduction (NH3-SCR) reaction over H–ZSM-5.