Deactivation and regeneration of TS-1/SiO₂ catalyst for epoxidation of propylene with hydrogen peroxide in a fixed-bed reactor

Abstract

TS-1/SiO₂ catalyst for the epoxidation of propylene with hydrogen peroxide in a fixed-bed reactor has been investigated. The catalyst activity decreases gradually with the online reaction time, but the selectivity of propylene epoxide is kept at about 93%. The fresh, deactivated and regenerated catalysts were characterized with X-ray diffraction, Fourier transform infrared spectroscopy, ultra-violet-visible diffuse reflectance, Brunner-Emmett-Teller method and thermogravimetric analysis, and the deactivated catalyst was regenerated with H₂O₂/methanol solution. Compared with the fresh catalyst, both the framework structure and the content of titanium in the framework of the deactivated and regenerated TS-1/SiO₂ catalysts were not changed. The major reason of the catalyst deactivation was the blockage of the channels of the catalyst by bulky organic by-products, which covered the active centers of titanium in TS-1. The deposited materials on the deactivated TS-1/SiO₂ catalyst could be removed by treatment with hydrogen peroxide/methanol solution or pure methanol; the higher the treatment temperature and the higher the concentration of H₂O₂ in methanol, the higher the extent of the regeneration. The regeneration treatment did not influence the product selectivity in the propylene epoxidation.

Key words： TS-1/SiO₂, epoxidation of propylene, fixed-bed reactor, deactivation; regeneration

Acknowledgments

This work has been supported by the Natural Science Foundation of China (Grant No. 21276183) and Program of Introducing Talents of Discipline to Universities (No. B06006).

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