Catalysis Today, Vol.243, 134-140, 2015
Epoxidation of bulky organic molecules over pillared titanosilicates
Layered and pillared TS-1 catalysts were prepared using surfactant C18H37-N+(CH3)(2)C6H12 -N+(CH3)(2)C6H13 in the hydroxide form as a structure directing agent and silicon(IV) ethoxide or its mixture with titanium(IV) butoxide as a pillaring medium. The pillaring treatment significantly increases the specific surface area (BET up to 685 m(2)/g) and thus the accessibility of active centres for bulky molecules. The addition of tetrabutylorthotitanate into the pillaring mixture has a positive effect on the material performance as a catalyst of cyclooctene, norbornene and alpha-pinene epoxidation under mild conditions, with hydrogen peroxide as the oxidant. Optimum composition of the pillaring medium is Si/Ti ratio 20. The highest yields of cyclooctene oxide (16.9% after 4h) and norbonene oxide (14.8% after 4.5 h) were obtained using the above-prepared catalyst at 60 degrees C with substrate/catalyst mass ratio being 10 and substrate/H2O2 ratio being 2. Selective oxidation of verbenol to verbenone was observed instead of the epoxidation with the above catalysts. (C) 2014 Elsevier B.V. All rights reserved.