In situ DRIFTS-MS studies on the oxidation of adsorbed NH3 by NOx over a Cu-SSZ-13 zeolite

Abstract

DRIFT spectroscopy combined with mass spectrometry was used to investigate the oxidation of adsorbed ammonia by NO2, NO + O-2 and NO2 + O-2 on a copper ion exchanged SSZ-13 (Cu-SSZ-13) zeolite. Compared with both NO2 and NO, the adsorption of ammonia is much stronger on the Cu-SSZ-13 zeolite. Two adsorbed ammonia species were found over the Cu-SSZ-13 zeolite studied here, notably ammonia on Bronsted acid sites (proton) and ammonia on Lewis acid sites (copper ions). These adsorbed ammonia species present different activity profiles and selectivity to N-2 during NH3 oxidation. The results obtained suggest that ammonia adsorbed onto copper ions in Cu-SSZ-13 is more active at low temperatures than proton-adsorbed NH3, and give rise to a higher selectivity to N-2. The formation of N2O is associated primarily with the reaction of NOx with proton-adsorbed NH3 via the formation and subsequent thermal decomposition of NH4NO3. Published by Elsevier B.V.