Unveiling the Mechanism of Cu-Support Interaction for Enhanced NH3-SCO Activity in Cu-Based Catalysts Supported on CeO2, Al2O3, and ZrO2
摘要
Ammonia-fueled internal combustion engines commonly exhibit significant unburned ammonia and ammonia slip, which critically impede the realization of their clean-combustion potential. The selective catalytic oxidation of ammonia (NH3-SCO) is considered an effective method for reducing emissions of unburned ammonia released from engines fueled by ammonia. In this study, Cu-based catalysts on CeO2, Al2O3, and ZrO2 were synthesized via the incipient-wetness impregnation technique, and their NH3-SCO activity was systematically evaluated using a simulated gas reaction system coupled with multiple physicochemical characterizations. The results demonstrated that Cu/CeO2 achieves 90% NH3 conversion in the temperature range of approximately 300–325 °C, showing superior activity compared with Cu/Al2O3 and Cu/ZrO2. For Cu/CeO2 and Cu/ZrO2, the Cu2+ species predominate and serve as the primary catalytic centers in NH3-SCO, whereas Cu/Al2O3 exhibits a higher fraction of Cu+. The smaller crystallites in Cu/CeO2 facilitated higher dispersion of the active species, whereas the excessive hydroxyl oxygen in Cu/ZrO2 inhibited catalytic activity. The enhanced Cu-support interaction in Cu/CeO2 contributes to higher concentrations of surface Oads and improves the redox behavior of CuO. The combined effect of these properties enhances NHx oxidation during the reaction, resulting in the superior catalytic performance observed for Cu/CeO2.
Graphical Abstract