Environmental Catalysis for NOx Reduction by Manipulating the Dynamic Coordination Environment of Active Sites.

Nowadays, it is challenging to achieve SO2-tolerant environmental catalysis for NOx reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO2. Herein, we achieve enhanced low-temperature SO2-tolerant NOx reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO2-CeO2 composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO2 support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO42- species in the presence of SO2. The low-coordinated Ce-SO42- species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH3 reactants. This work proposes a new notion to improve the SO2 resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO2-tolerant environmental catalysis in practical applications.