Role of the different copper species on the activity of Cu/zeolite catalysts for SCR of NOx with NH3

• Published in: Applied catalysis. B, Environmental Vol. 147; pp. 420 - 428
• Main Authors: Pereda-Ayo, Beñat, De La Torre, Unai, Illán-Gómez, María José, Bueno-López, Agustín, González-Velasco, Juan R.
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 05.04.2014
• Subjects: ACTIVITY; Catalysis; CATALYSTS; Copper; COPPER OXIDE; Cu cluster; Cu-zeolite; Emission analysis; Inductively coupled plasma; NITROGEN OXIDE; NOx removing; SCR; Spectroscopy; X RAY SPECTROSCOPY; X-ray photoelectron spectroscopy; Zeolites; SCR; Cu-zeolite; Cu cluster; NOx removing
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2013.09.010

•NH3 NOx-SCR is studied on Cu-ZSM5 and Cu-BETA prepared by ion exchange and impregnation.•CuO and Cu(II) exchanged on tetrahedral and octahedral positions of zeolite framework were found.•CuO prevails in high Cu-content on ZSM5. Isolated Cu(II) ions prevail in low Cu-content on BETA catalysts.•CuO promotes NOx reduction at low temperature.•Isolated Cu(II) ions maintain high NOx conversion at high temperatures. The SCR of NOx with NH3 has been studied by using different Cu zeolite catalysts, prepared both with ZSM5 and BETA zeolite supports by ionic exchange or by impregnation. The catalysts were characterized by ICP-AES, N2 adsorption at −196°C, XRD, TEM, XPS and H2-TPR. The catalysts characterization confirmed the presence of different Cu(II) species on all catalyst (CuO and Cu(II) exchanged on tetrahedral and octahedral positions of the zeolites framework). Clear evidences of Cu(I) or Cu(0) species were not obtained. CuO was more abundant in high copper-content catalysts and in ZSM5 catalysts, due to its lower ionic exchange capacity, while isolated Cu(II) ions are more abundant in low copper-content catalysts and in BETA catalysts. It was concluded that CuO catalyzes the oxidation of NO to NO2, and this favors the reduction of NOx at lower temperature (the NH3-NO2 reaction is faster than the NH3-NO reaction because NO2 is much more oxidizing than NO), whereas isolated Cu(II) ions maintain high NOx conversion at high temperatures.