The promotion effect of manganese on Cu/SAPO for selective catalytic reduction of NOx with NH3

Abstract

The activity and hydrothermal stability of Cu/SAPO and xMn–2Cu/SAPO for low-temperature selective catalytic reduction of NO_x with ammonia were investigated. An ion-exchanged method was employed to synthesize xMn–2Cu/SAPO, which was characterized by N₂ adsorption, ICP-AES, X-ray diffraction (XRD), NH₃-temperature programmed desorption (NH₃-TPD), NO oxidation, X-ray photoelectron spectrum (XPS), UV-vis, H₂-temperature programmed reduction (H₂-TPR) and diffuse reflectance infrared Fourier transform spectra (DRIFTS). 2Mn–2Cu/SAPO and 4Mn–2Cu/SAPO showed the best SCR activity, in that at 150 °C NO conversion reached 76% and N₂ selectivity was above 95% for the samples. NO oxidation results showed that the 2Mn–2Cu/SAPO had the best NO oxidation activity and the BET surface area decreased as manganese loading increased. XRD results showed that the metal species was well dispersed. NH₃-TPD showed that the acid sites have no significant influence on the SCR activity of xMn–2Cu/SAPO. H₂-TPR patterns showed good redox capacity for xMn–2Cu/SAPO. UV-vis and H₂-TPR showed that the ratio of Mn⁴⁺ to Mn³⁺ increased as manganese loading increased. XPS spectra showed a significant amount of Mn³⁺ and Mn⁴⁺ species on the surface and addition of manganese increased the ratio of Cu²⁺. The promotion effect of manganese to 2Cu/SAPO comes from the generation of Mn³⁺ and Mn⁴⁺ species. Deduced from the DRIFTS spectra, the Elay–Rideal mechanism was effective on 4Mn–2Cu/SAPO.