Nature of Cu Species in Cu–SAPO-18 Catalyst for NH3–SCR: Combination of Experiments and DFT Calculations

A series of Cu–SAPO-18 catalysts with various Cu loadings were prepared and their catalytic activities were tested for the selective catalytic reduction of NO with NH3. The catalysts were characterized by means of XRD, N2 adsorption–desorption, TEM, XPS, UV–vis DRS, H2-TPR, NH3-TPD and EPR. Isolated Cu2+ ions are confirmed to be the catalytic active sites. Cu-4.42 catalyst exhibits high NO conversion (>80%) at the lowest temperature of 200 °C among all catalysts. It can be attributed to the maximum amount of isolated Cu2+ ions in Cu-4.42 catalyst. DFT calculations show that the isolated Cu ions are located in the pear shaped cavity and exhibit a preference for the neighboring of 6R planes of Cu–SAPO-18. NH3–SCR mechanism over Cu–SAPO-18 catalyst is elucidated by a combination of in situ DRIFTS technique and DFT calculations, in which the dissociation of NH3 and the oxidation of NO are shown to be key steps in the reaction.