Ru(II)-diimine complexes have been the class of metal complexes the most deeply investigated due to their unique photophysical and chemical properties. Our laboratory leveraged their use to initiate various redox events in cytochrome P450 enzymes and harness their synthetic potential upon visible light excitation. These heme-thiolate enzymes activate molecular dioxygen using two reducing equivalents to carry out selective C-H functionalization on a wide range of organic substrates. Rational and directed evolution approaches have been employed to engineer libraries of light-driven hybrid enzymes with enhanced photocatalytic activity and substrate scope. In addition, we have recently explored several chemoenzymatic approaches by combining the advantages of chemical catalysts with the regio and stereoselectivity of the P450 biocatalysts. We reported strategies to access trifluoromethylated substituted arenes and biaryl alkanoic acids that could be further oxyfunctionalized by a variety of P450 enzymes.

On the use of Ru(II)-diimine complexes to harness cytochrome P450 synthetic potential

ACS Spring 2022

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