Recognizing zeolite topologies for Cu²⁺ localizations with effective activities for selective catalytic reduction of...

Cu-loaded zeolites are widely investigated in selective catalytic reduction of nitrogen oxide, but effects of zeolite topologies on formed active species and the changing tendency remain unexplored. In this work, catalytic turnover frequencies (TOF) of Cu loaded ZSM-5, Beta, MOR, and SSZ-13 were first determined. The topology-localized Cu species in these zeolites were analyzed by temperature-programmed reduction of H₂. Then Multiple Linear Regression distinguished TOF contributions (k_j, s^-1·mol^-1) of the Cu species. Density functional theory calculated NH₃ dehydrogenation energy of the Cu species. As a result, topologies with more node atoms showed bigger k_j and lower dehydrogenation energies simultaneously. The best topology in each zeolite was 10-membered ring (ZSM-5), 6-membered ring facing a 12-membered ring (Beta), 8-membered ring (MOR), and cha cage (SSZ-13). Moreover, cha cage-localized Cu²⁺ exhibited the largest k_j and the lowest dehydrogenation energy among all the Cu species. This work reveals topology-catalysis relationships in the zeolite, which benefits zeolite design for enhanced catalytic performances.