Process for light-driven hydrocarbon oxidation at ambient temperatures
AssigneeThe United States of America as represented by the United States Department of Energy
InventorJohn A. Shelnutt
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Abstract
A photochemical reaction for the oxidation of hydrocarbons uses molecular oxygen as the oxidant. A reductive photoredox cycle that uses a tin(IV)- or antimony(V)-porphyrin photosensitizer generates the reducing equivalents required to activate oxygen. This artificial photosynthesis system drives a catalytic cycle, which mimics the cytochrome P.sub.450 reaction, to oxidize hydrocarbons. An iron(III)- or manganese(III)-porphyrin is used as the hydrocarbon-oxidation catalyst. Methylviologen can be used as a redox relay molecule to provide for electron-transfer from the reduced photosensitizer to the Fe or Mn porphyrin. The system is long-lived and may be used in photo-initiated spectroscopic studies of the reaction to determine reaction rates and intermediates.
Claims20
A method for oxidizing hydrocarbons in a catalytic cycle that is driven by a photo-redox cycle that mimics photosynthesis which comprises the steps of:
- providing a solution comprising a metalloporphyrin photosensitizer that generates reducing equivalents for activating oxygen, a biomimetic hydrocarbon-oxidation catalyst, molecular oxygen as the oxidant, a hydrocarbon substrate molecule, a sacrificial electron donor, an acylating agent, and a solvent;
- and
- irradiating said solution with light in the presence of molecular oxygen.
Dependencies are inferred from the claim text.