Ammonia removal in selective catalytic oxidation: Influence of catalyst structure on the nitrogen selectivity.

Abstract

Selective catalytic oxidation is regarded as an effective and favored method for the removal of hazardous ammonia. A number of M-Pt/USY (M=Mn, Fe, Ce and Pr) catalysts were prepared and the resulting materials were characterized using N2 adsorption/desorption, XRD, TEM, NH3-TPD, XPS and H2-TPR. It was found that the addition of non-stoichiometric metal oxides to Pt/USY leads to the generation of additional acid sites for ammonia chemisorption and that N2 selectivity improved with increased strong acidity of the bi-functional catalysts. The oxidation state of active Pt could be adjusted by the introduction of non-stoichiometric metal oxides with increased concentrations of oxidized Ptδ+ species observed in the order of FeOx >CeO2-x >MnO2-x >Pr6O11. High valence platinum surrounded by atomic oxygen that can act as a proton scavenger to drive ammonia activation, inhibiting O2 dissociation and therefore improve N2 selectivity. Fe-containing USY zeolite is demonstrated to be a preferred catalyst for the removal of ammonia, due to its high N2 selectivity and good hydrothermal stability.