Evolution of copper species on Cu/SAPO-34 SCR catalysts upon hydrothermal aging

Cu-modified SAPO-34 molecular sieves with different Cu loading amounts were prepared by ion-exchange and impregnation methods. Both series of catalysts were hydrothermally treated at 750   °C in 10   vol% H 2 O/air for 24   h. The catalysts were characterized by inductively coupled plasma optical emission spectrometry (ICP-OES), electron paramagnetic resonance (EPR), X-ray photoelectron spectroscopy (XPS), H 2 temperature-programmed reduction (H 2 -TPR), NH 3 temperature-programmed desorption (NH 3 -TPD) and diffused reflectance infrared flourier transform spectroscopy (DRIFTS). All the fresh catalysts show high activity toward the selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) at low temperatures regardless of preparation method. Generally, the hydrothermal aging shifts the operation window of the catalysts towards high temperatures. The improvement in high-temperatures activity is attributed to the migration of surface CuO clusters into the ion-exchanged sites as isolated Cu 2+ during ageing, which suppresses the competitive oxidation of NH 3 . The loss of low-temperatures activity is also related to the decrease in the amount of active surface CuO clusters, inhibiting the oxidation of NO to NO 2 and fast SCR reaction. Interestingly, the amount of Lewis acid sites increase linearly with the increasing isolated Cu 2+ , while the Brønsted acidity is weakened.