Oxidation of cyclohexane using a novel RuO2–zeolite nanocomposite catalyst

Abstract

We report the synthesis, using an organic-template-free hydrothermal crystallization method, and catalysis of a new type of nanocomposite material, 1.3 nm-sized RuO2 particles confined in faujasite zeolite. The zeolite-confined RuO2 composites were fully characterized with X-ray powder diffraction, Ru K-edge X-ray absorption, and high-resolution transmission electron microscopy. XRD and X-ray fluorescence analysis indicate that the framework is faujasite zeolite with a Si:Al ratio of 1.25. Ru K-edge X-ray absorption near-edge structures indicate that the ruthenium species in the zeolite is Ru(IV) with nearest-neighbor octahedral environments similar to hydrous RuO2, i.e., distorted "RuO6". The k2-weighted extended X-ray absorption fine structure indicates that the Ru(IV) species anchored in the zeolite likely form amorphous RuO2 with a 2D-chain structure, in which RuO6 units are connected together by two shared oxygen atoms. TEM shows that the particle size of RuO2 encapsulated inside the supercages of FAU is about 1.3 nm. The RuO2–FAU composites display significant catalytic activity in the oxidation of cyclohexane with tBHP under mild (room temperature and 1 atm (1 atm [Formula: see text] 101.325 kPa)) conditions. The ketone and alcohol concentration can be as high as 0.26 mol L–1 in 5 h with 48% peroxide efficiency. The catalyst is stable and reusable. Possible oxidation mechanisms are also discussed.Key words: nanocomposite, ruthenium oxide, catalysis, oxidation, zeolite.