Polybrominated diphenyl ethers (PBDEs) have recently become the subject of many studies due to their potent bioactivities such as anti-MRSA activities. Metabolites structurally related to PBDEs have been isolated from Pseudoalteromonas living in association with nudibranchs. Cytochrome P450 (CYP) is a ubiquitous enzyme with remarkably diverse catalytic activities and they have been the target of many directed evolution studies for innovative chemistries. In this study, the marine marine bacterial CYP involved in the biosynthesis of bioactive PBDE metabolites is being engineered to catalyze Ullmann-type coupling necessary to connect labile aromatic moieties to aid in the synthesis of medicinally important molecules. . Such linkage is a challenging bond to form by the conventional synthetic means and will contribute to more expedient and greener development of novel medicines.. Herein presented are our efforts toward engineering of the CYP through chemical random mutagenesis, a method that may be more easily adapted by the organic synthetic community than PCR-based methods.

Directed evolution through chemical mutagenesis towards biocatalysts in natural product synthesis

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