An Efficient Light-Driven P450 BM3 Biocatalyst

被引:114
作者
Ngoc-Han Tran [1 ]
Daniel Nguyen [1 ]
Dwaraknath, Sudharsan [1 ]
Mahadevan, Sruthi [1 ]
Chavez, Garrett [1 ]
Angelina Nguyen [1 ]
Thanh Dao [1 ]
Mullen, Sarah [1 ]
Thien-Anh Nguyen [1 ]
Cheruzel, Lionel E. [1 ]
机构
[1] San Jose State Univ, Dept Chem, San Jose, CA 95192 USA
基金
美国国家科学基金会;
关键词
ELECTRON-TRANSFER; CYTOCHROME-P450; ACTIVATION; HYDROXYLATION; CHEMISTRY; CATALYSIS; OXIDATION; CYP102A1; ENZYMES;
D O I
10.1021/ja409337v
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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/miri).
引用
收藏
页码:14484 / 14487
页数:4
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