Selective catalytic oxidation of ammonia over nano Cu/zeolites with different topologies

The selective catalytic oxidation of ammonia (NH3-SCO) is the last mitigation step in exhaust treatment using a 4-way catalytic converter to convert any excess and unreacted NH3 (that was used as a reductant of NOx) into environmentally benign N-2 and H2O. Here, we report a series of highly reactive and selective nano Cu/zeolites for the NH3-SCO reaction. The NH3-SCO activity was found in the order nano Cu/ZSM-5 (MFI topology) > Cu/Beta (BEA) > Cu/MCM-49 (MWW) > Cu/Y (FAU) > Cu/Mordenite (MOR) > Cu/Ferrierite (FER). The best catalyst, i.e., nano Cu/ZSM-5, achieves 98% NH3 conversion at 250 degrees C with the N-2 yield maintained at >98% even at up to 500 degrees C. When assessed under practical exhaust conditions in the presence of moisture (5% H2O) as well as that after hydrothermal aging (5% H2O, 850 degrees C, 8 h), the nano Cu/ZSM-5 exhibited only minor deactivation as a result of its good retention of Cu dispersion, pore structure and specific surface area. Furthermore, small micropore (10-membered ring, 10-MR) topologies were found to be crucial in maintaining high N-2 yields. For Cu/Y and Cu/Mordenite, composed of 12-MR pores that are non-interconnected with smaller pores, their N-2 yields were compromised by forming NOx at temperatures above 400 degrees C. Based on the in situ DRIFTS study, the iSCR mechanism appears to be applicable for all fresh and aged Cu/zeolites with the exception of fresh Cu/MCM-49 that follows the imide mechanism.