Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Ligands
Nitrene Transfer Catalyzed by a Non-Heme Iron Enzyme and Enhanced by Non-Native Small-Molecule Ligands
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DOI：
10.1021/jacs.9b11608
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发表时间：
2019-12-18
影响因子：
15
通讯作者：
Arnold, Frances H.
中科院分区：
文献类型：
--
作者：
Goldberg, Nathaniel W.;Knight, Anders M.;Arnold, Frances H.
过渡金属催化是构建化学键的有力工具。在这里，我们表明，假单胞菌savastanoi乙烯形成酶，非血红素铁酶，可以催化烯烃氮杂环丙烷化和氮烯C-H插入，这些活动可以通过定向进化得到改善。非血红素铁中心允许通过添加金属配位分子来容易地修饰初级配位球，从而能够使用小分子控制酶活性和选择性。
Transition-metal catalysis is a powerful tool for the construction of chemical bonds. Here we show that Pseudomonas savastanoi ethylene-forming enzyme, a non-heme iron enzyme, can catalyze olefin aziridination and nitrene C-H insertion, and that these activities can be improved by directed evolution. The non-heme iron center allows for facile modification of the primary coordination sphere by addition of metal-coordinating molecules, enabling control over enzyme activity and selectivity using small molecules.