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An Efficient Light-Driven P450 BM3 Biocatalyst

2013; American Chemical Society; Volume: 135; Issue: 39 Linguagem: Inglês

10.1021/ja409337v

1943-2984

Ngoc-Han Tran, Daniel Nguyen, Sudharsan Dwaraknath, Sruthi Mahadevan, Garrett Chavez, Angelina Nguyen, Thanh Dao, Sarah Mullen, Thien-Anh Nguyen, Lionel Cheruzel,

Metal-Catalyzed Oxygenation Mechanisms

P450s are heme thiolate enzymes that catalyze the regio- and stereoselective functionalization of unactivated C-H bonds using molecular dioxygen and two electrons delivered by the reductase. We have developed hybrid P450 BM3 heme domains containing a covalently attached Ru(II) photosensitizer in order to circumvent the dependency on the reductase and perform P450 reactions upon visible light irradiation. A highly active hybrid enzyme with improved stability and a modified Ru(II) photosensitizer is able to catalyze the light-driven hydroxylation of lauric acid with total turnover numbers of 935 and initial reaction rate of 125 mol product/(mol enzyme/min).