Facile synthesis of Ag-CuO/SBA-15 for aerobic epoxidation of olefins with high activity

Abstract

An efficient ‘structure-property’ catalyst Ag-CuO/SBA-15 for aerobic epoxidation of olefins was designed and prepared via a simple grinding method, which provided a dynamic assembly driving force to push the precursors into the channels step by step. Partial melting on the precursor particles surface is necessary for synthesizing the Ag-CuO/SBA-15 catalysts. During the thermal grinding process, the partial melting Cu(NO3)2 first adhered on AgNO3 particles surface because the N of AgNO3 possess stronger interaction with Cu(NO3)2 than OH- of SBA-15, then the mixture of melting precursors on AgNO3 particles surface were sucked into the channels of SBA-15 step by step. Finally, high dispersion of both Ag and CuO nanoparticles were formed in the SBA-15 channels after calcination. The interaction between Ag and CuO, which was characterized by high-resolution transmission electron microscopy, UV–vis and x-ray powder diffraction, enhances the catalytic activity of the catalysts, giving high conversion and selectivity to the epoxides. The reaction mechanism is as follows, the solvent xylene molecule was first oxidized on the Ag surface to form methyl-benzaldehyde (R1), and then moved to the CuO surface to form the peroxidic radical (R2), the peroxidic radical attacked the trans-stilbene C=C bonds on the CuO surface to obtain the epoxides. This synergistic effect shows high activity toward the epoxidation of trans-stilbene.