The effects of impregnation of precious metals on the catalytic activity of titanium silicate (TS-1) in epoxidation of propene using hydrogen peroxide

Abstract

Propene oxide is an important chemical intermediate and titanium silicalite (TS-1) has been widely investigated as a promising catalyst for the direct epoxidation of propene with ex-situ or in-situ produced hydrogen peroxide as an oxidant. In order to clarify the effects of the kind of precious metal and treatment process in the catalyst preparation on the propene epoxidation and the hydrogen peroxide decomposition, TS-1 was impregnated with gold and palladium via drying, calcination and reduction and the experiments to check its catalytic performance were conducted in a gas aspirating autoclave reactor in the absence of mass transfer limitations. The presence of precious metals vigorously catalyzed the side reactions and hydrogen peroxide decomposition. Some of the precious metal containing TS-1 catalysts showed high initial rates but there was no catalyst with a propene oxide yield after 5h reaction time comparable to TS-1 alone because of the enhancement of side reactions by precious metals. The significant decline in the selectivity to propene oxide over the dried precious metal containing TS-1 catalysts was attributed to the leaching of precious metals into the reaction medium. Palladium containing TS-1 showed exceptionally high decomposition of hydrogen peroxide. Reduction and calcination increased the decomposition by forming metallic gold and palladium. Homogeneous dispersion of gold nanoparticles was achieved by a sol immobilization method which led to a decrease of propene oxide selectivity and an increase of hydrogen peroxide decomposition.