Cytochrome P450s are heme-thiolate enzymes that activate molecular dioxygen to carry out selective oxyfunctionalization of a wide range of organic substrates. Our laboratory has utilized the photochemical properties of Ru(II)-diimine photosensitizers to activate several P450 enzymes upon visible light excitation. A combination of rational and directed evolution approaches has enabled the engineering of the next generation of light-driven hybrid enzymes in order to enhance their photocatalytic activity and substrate scope. In addition, the tunability and derivatization of the inorganic complexes have promoted the formation of dimeric structures and heterogeneous biocatalysts and provided insights into the rate-limiting steps in the light-driven hybrid P450 enzyme. We recently turned our attention to the development of chemoenzymatic approaches to capitalize on the merging of chemical catalysis and P450 biocatalysis. Building on a selective light-driven trifluoromethylation /oxyfunctionalization of several substituted arenes, we recently developed a one-pot chemoenzymatic approach to access various high added value compounds.

Ru(II)-diimine complexes coupled with P450 enzymes

ACS Spring Meeting 2021

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