DEVELOPMENT OF HIGH PERFORMANCE INTEGRATED CATALYSTS FOR SUSTAINABLE CHEMICAL TRANSFORMATION SYSTEMS

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In this research project, we aimed development of high performance integrated catalysts for environmentally-friendly and sustainable materials conversion systems. The target reactions are (1) oxidation reactions using molecular oxygen and/or water, and (2) selective carbon-carbon bond formation reactions, which are highly important for synthesis of finechemicals. We have developed novel nanostructured heterogeneous catalysts capable of cooperative activation by several active species, using inorganic crystallites, e. g., hydroxyapatites (HAPs), hydrotalcites (HTs), and montmorillonites (monts), as unique supports. As for the alcohol oxidation, RuHAP functionalized Fe_2O_3 nanoparticles was prepared, which showed extremely high activity fort aerobic alcohol oxidation and also acted as magnetically recoverable catalyst. Furthermore, highly active HT catalyst for conversion of cyclohexanol to cyclohexanone, which is known as difficult oxidation, could be developed. Recent interest in the … More alcohol oxidation has been dehydrogenation without using any oxidants. The Ag/HT catalyst could be extremely high activity for the dehydrogenation of various alcohols. The surface basicity of the HT and the Ag nanoparticles formed on the HT showed the concerted activation of alcohols and generated hydrogen quatitatively. Utilities of the HT catalysts were expanded to hydration of nitrile to amide using vanadium supported HT. Interestingly, acidic clay materials of montmorillonites could be used as solid acid catalysts having protons or various metal cations. These solid acids could catalyze addition reaction of various nucleophiles to olefins forming various C-C, C-O, and C-N bonds.These integrated catalysts can be easily prepared and exhibit outstanding performances, which open a new avenue for sustainable green organic syntheses. The prominent catalyst behavior for the above transformations is focused in relation to the concerted functions between the surface properties of the inorganic crystallites and the metal active species. Less