title: An efficient light-driven P450 BM3 biocatalyst.
abstract: 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).
authors.affiliation: Department of Chemistry, San José State University , One Washington Square, San José, California 95192-0101, United States.
authors.forename: Ngoc-Han
authors.initials: NH
authors.lastname: Tran
authors.forename: Daniel
authors.initials: D
authors.lastname: Nguyen
authors.forename: Sudharsan
authors.initials: S
authors.lastname: Dwaraknath
authors.forename: Sruthi
authors.initials: S
authors.lastname: Mahadevan
authors.forename: Garrett
authors.initials: G
authors.lastname: Chavez
authors.forename: Angelina
authors.initials: A
authors.lastname: Nguyen
authors.forename: Thanh
authors.initials: T
authors.lastname: Dao
authors.forename: Sarah
authors.initials: S
authors.lastname: Mullen
authors.forename: Thien-Anh
authors.initials: TA
authors.lastname: Nguyen
authors.forename: Lionel E
authors.initials: LE
authors.lastname: Cheruzel
mesh_terms: D001410:Bacillus megaterium / Q000201:enzymology*; D001426:Bacterial Proteins / Q000737:chemistry* / Q000378:metabolism; D056831:Coordination Complexes / Q000737:chemistry* / Q000378:metabolism; D003577:Cytochrome P-450 Enzyme System / Q000737:chemistry* / Q000378:metabolism; D004795:Enzyme Stability; D006418:Heme / Q000737:chemistry / Q000378:metabolism; D006900:Hydroxylation; D007850:Lauric Acids / Q000378:metabolism; D008027:Light; D008958:Models, Molecular; D009251:NADPH-Ferrihemoprotein Reductase / Q000737:chemistry* / Q000378:metabolism; D017319:Photosensitizing Agents / Q000737:chemistry* / Q000378:metabolism; D012428:Ruthenium / Q000737:chemistry* / Q000378:metabolism
chemical_list: D001426:Bacterial Proteins; D056831:Coordination Complexes; D007850:Lauric Acids; D017319:Photosensitizing Agents; C030358:lauric acid; D006418:Heme; D012428:Ruthenium; D003577:Cytochrome P-450 Enzyme System; D009251:NADPH-Ferrihemoprotein Reductase; C052423:flavocytochrome P450 BM3 monoxygenases
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