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| - Hydroformylation of 1-Hexene inSupercritical Carbon Dioxide: Characterization, Activity, andRegioselectivity Studies
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| - The hydroformylation of alkenes is a major commercialprocess used for the production of oxygenated organiccompounds. When the hydroformylation reaction is performedusing a homogeneous catalyst, an organic or aqueoussolvent is employed, and a significant effort must be expendedto recover the catalyst so it can be recycled. Developmentof a selective heterogeneous catalyst would allowsimplification of the process design in an integratedsystem that minimizes waste generation. Recent studieshave shown that supercritical carbon dioxide (scCO2) as areaction solvent offers optimal environmental performanceand presents advantages for ease of product separation.In particular, we have considered the conversion of 1-hexeneto heptanal using rhodium- and platinum-phosphinecatalysts tethered to supports insoluble in scCO2 todemonstrate the advantages and to understand the limitationsof a solid-catalyzed process. One of the historicallimitations of supported catalysts is the inability to controlproduct regioselectivity. To address this concern, wehave developed tethered catalysts with phosphinated silicaand controlled pore size MCM-41 and MCM-20 supportsthat provide improved regioselectivity and conversion relativeto their nonporous equivalents. Platinum catalystssupported on MCM-type supports were the most regioselective whereas the analogous rhodium catalysts werethe most active for hydroformylation of 1-hexene in scCO2.
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