PNNL

Abstract

Cu-SSZ-13 catalysts with various Cu loadings were prepared via solution ion exchange. The hydrated samples were studied with Electron Paramagnetic Resonance (EPR). Cu2+ ion coordination numbers were obtained by analyzing the hyperfine structures while Cu-Cu distances were estimated from line broadening of the EPR features. By coupling EPR and temperature-programmed reduction (TPR) results, two Cu2+ ion locations were suggested. Standard and fast NH3-SCR, as well as non-selective NH3 oxidation reactions were carried out over these catalysts at high space velocities. For the SCR reaction, intra-particle diffusion limitation was found throughout the reaction temperatures investigated. Although clear structure-activity relationships cannot be derived, the reaction results allow for reactant diffusivities and Cu2+ ion locations to be estimated. The slower NH3 oxidation reaction, on the other hand, is kinetically limited at low temperatures, and, therefore, allows for a correlation between Cu2+ ion location and reaction kinetics to be made. Furthermore, the dynamic Cu2+ ion motion as a function of temperature could also be derived from the NH3 oxidation kinetics.