Activity, propene poisoning resistance and hydrothermal stability of copper exchanged chabazite-like zeolite catalysts for SCR of NO with ammonia in comparison to Cu/ZSM-5

Copper, iron, and mixed copper/iron exchanged zeolites containing ZSM-5 and chabazite-like zeolites (SSZ-13, SAPO-18 and SAPO-34) were studied for selective catalytic reduction (SCR) of NO with NH3 with or without propene. Cu/ZSM-5, Cu/SSZ-13, Cu/SAPO-18 and Cu/SAPO-34 exhibited high NO conversions without propene. However, as compared to Cu/ZSM-5, NO conversions over Cu/SSZ-13, Cu/SAPO-18 and Cu/SAPO-34 were more stable with propene, due to coke formation over Cu/ZSM-5. The results of N-2-adsorption/desorption and XPS showed that the surface area, Cu+/Cu2+ ratio and the surface amount of Cu content of Cu/ZSM-5 catalysts changed from 324 m(2)/g, 0.03 and 11.5 wt% for the fresh Cu/ZSM-5 catalyst to 68 m(2)/g, 0.34 and 5.3 wt% for the used sample. However, there were little changes between fresh and used Cu/SSZ-13, Cu/SAPO-18 and Cu/SAPO-34 catalysts. Moreover, Cu/ZSM-5 catalyst showed a larger decline in NO conversion with time on stream and a higher adsorption amount of propene compared to Cu/SSZ-13, Cu/SAPO-18 and Cu/SAPO-34 catalysts. The resistance to hydrocarbon poisoning depended on the pore geometry of the zeolites. During NH3-SCR, the presence of medium-pore sizes in Cu/ZSM-5 led to hydrocarbon deposition, which blocked the active sites and also decreased the active intermediates needed for NO conversion. Cu/SSZ-13, Cu/SAPO-18 and Cu/SAPO-34 catalysts, on the other hand, with small pores and cage diameters and with one-dimensional channel structures, showed higher hydrocarbon poison resistance. Moreover, these copper exchanged small-pore zeolites showed much higher hydrothermal stability than the medium-pore Cu/ZSM-5. (C) 2012 Elsevier B.V. All rights reserved.