Mechanistic Investigation of Oxygen Rebound in a Mononuclear Nonheme Iron Complex

被引：18
|
作者：
Pangia, Thomas M. [1 ]
Yadav, Vishal [1 ]
Gerard, Emilie F. [2 ,3 ]
Lin, Yen-Ting [2 ,3 ]
de Visser, Sam P. [2 ,3 ]
Jameson, Guy N. L. [4 ]
Goldberg, David P. [1 ]
机构：
[1] Johns Hopkins Univ, Dept Chem, 3400 North Charles St, Baltimore, MD 21218 USA
[2] Univ Manchester, Manchester Inst Biotechnol, 131 Princess St, Manchester M1 7DN, Lancs, England
[3] Univ Manchester, Sch Chem Engn & Analyt Sci, 131 Princess St, Manchester M1 7DN, Lancs, England
[4] Univ Melbourne, Mol Sci & Biotechnol Inst Bio21, Sch Chem, 30 Flemington Rd, Parkville, Vic 3010, Australia
来源：
INORGANIC CHEMISTRY | 2019年 / 58卷 / 15期
基金：
英国生物技术与生命科学研究理事会;
关键词：
KETOGLUTARATE DIOXYGENASE TAUD; C-H HYDROXYLATION; ALIPHATIC HALOGENASE; OXIDATION; REACTIVITY; PHENOLS; CYTOCHROME-P450; IRON(IV)-OXO; INSIGHTS; TAURINE;
D O I：
10.1021/acs.inorgchem.9b01208
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
An iron(III) methoxide complex reacts with para-substituted triarylmethyl radicals to give iron(II) and methoxyether products. Second-order rate constants for the radical derivatives were obtained. Hammett and Marcus plots suggest the radical transfer reactions proceed via a concerted process. Calculations support the concerted nature of these reactions involving a single transition state with no initial charge transfer. These findings have implications for the radical "rebound" step invoked in nonheme iron oxygenases, halogenases, and related synthetic catalysts.
引用
收藏
页码：9557 / 9561
页数：5
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