Abstract
A series of Cd modified titanium silicalite 1 catalysts with different Cd content (xCd-TS-1, x=1–15) were successfully prepared by ultrasound impregnation. Epoxidation of butadiene over these catalysts were investigated using hydrogen peroxide as oxidant, which indicated that Cd greatly improve the catalytic performance of TS-1 and the selectivity of epoxide. Various characterization methods including quantum chemical calculation were employed to explore the specific roles of Cd in promoting TS-1 catalytic activity. Theoretical calculation consistently suggested TiO bond were weakened owing to the introduction of Cd, which resulted in the structure of Cd-TS-1 becoming more relaxant. As a consequence, it is favorable to methanol solvent and H2O2 interacting with the Ti active site to form five-member transition state during reaction. It was observed that catalysts modified with 1–5wt% Cd presented both high catalytic activity and good reusability. The highest yield of 0.63mol/L of vinyloxirane (VO) was obtained, while turnover number (TON, determined as the molar VO obtained per molar Ti atom) could reach to 1466.
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