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Activities of Polyhedral Vanadium-Containing Silsequioxane-Based Catalysts for Photo-Assisted Oxidation of Hydrocarbons

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The catalytic activity of a polyhedral vanadium-containing silsesquioxane ((c-C5H9)7Si7O12VO, 1b) with a cubic core structure towards the selective photooxidation of benzene, cyclohexane, and adamantane was examined under O2 (1 atm) at around 300 K. The reaction of benzene in the presence of 1b afforded phenol selectively, but the TON was low (~ 1.4). Complex 1b showed high activity towards the reaction of cyclohexane (TON~16) and adamantane (TON ~7.0). The order of the reactivity of the C-H bonds in adamantane was tertiary C-H > secondary C-H. In addition to 1b, the mixtures of vanadyl bisacetylacetonate and incompletely-condensed silsesquioxanes with silanol functionality showed relatively high activities, although vanadyl bisacetylacetonate itself was not effective. The degradation of the catalysts in the course of the reaction was partly suppressed in the presence of molecular sieves-4A.

Affiliations: 1: Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Sakyo-ku, Kyoto 606-01 Japan


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