Crystallographic and spectroscopic characterization of a nonheme Fe(IV)=O complex

被引:797
作者
Rohde, JU
In, JH
Lim, MH
Brennessel, WW
Bukowski, MR
Stubna, A
Münck, E
Nam, W
Que, L
机构
[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[2] Univ Minnesota, Ctr Met Biocatalysis, Minneapolis, MN 55455 USA
[3] Ewha Womans Univ, Dept Chem, Seoul 120750, South Korea
[4] Ewha Womans Univ, Div Mol Life Sci, Seoul 120750, South Korea
[5] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
关键词
D O I
10.1126/science.299.5609.1037
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Following the heme paradigm, it is often proposed that dioxygen activation by nonheme monoiron enzymes involves an iron(IV)=oxo intermediate that is responsible for the substrate oxidation step. Such a transient species has now been obtained from a synthetic complex with a nonheme macrocyclic ligand and characterized spectroscopically. Its high-resolution crystal structure reveals an iron-oxygen bond length of 1.646(3) angstroms, demonstrating that a terminal iron(IV)=oxo unit can exist in a nonporphyrin ligand environment and [ending credence to proposed mechanisms of nonheme iron catalysis.
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页码:1037 / 1039
页数:3
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