Impact of copper loading on nh3-selective catalytic reduction, oxidation reactions and N2O formation over Cu/SAPO-34

Abstract

We developed a procedure for aqueous ion exchange to obtain different Cu loadings of Cu/SAPO-34 (between 0 and 2.6 wt %). The catalysts were washcoated on monoliths and characterised with respect to their activity and selectivity under standard selective catalytic reduction (SCR), fast SCR, NH3 oxidation and NO oxidation reactions. They were further characterised using X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), H2-temperature programmed reduction (H2-TPR), ultraviolet (UV)-vis spectroscopy and NH3 adsorption. As expected, activity of all reactions increased with copper loading, due to increased number of active sites. However, the N2O formation during standard and fast SCR yielded interesting mechanistic information. We observed that N2O formation at low temperature increased with copper loading for the standard SCR reaction, while it decreased for fast SCR. The low-temperature N2O formation during fast SCR thus occurs predominantly over Brønsted sites. Species responsible for N2O formation during standard SCR, on the other hand, are formed on the copper sites. We further found that the fast SCR reaction occurs to a significant extent even over the H/SAPO-34 form. The Brønsted sites in SAPO-34 are thus active for the fast SCR reaction.