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（19）由大环配体支撑的羧酸根桥联二铁（II）配合物中配体动力学的F NMR研究

(19)F NMR study of ligand dynamics in carboxylate-bridged diiron(II) complexes supported by a macrocyclic ligand.

作者信息

Minier Mikael A, Lippard Stephen J

机构信息

Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.

出版信息

Dalton Trans. 2015 Nov 7;44(41):18111-21. doi: 10.1039/c5dt02138c. Epub 2015 Sep 29.

DOI:10.1039/c5dt02138c
PMID:26418547
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC4618381/
Abstract

A series of asymmetrically carboxylate-bridged diiron(ii) complexes featuring fluorine atoms as NMR spectroscopic probes, [Fe2(PIM)(Ar(4F-Ph)CO2)2] (10), [Fe2(F2PIM)(Ar(Tol)CO2)2] (11), and [Fe2(F2PIM)(Ar(4F-Ph)CO2)2] (12), were prepared and characterized by X-ray crystallography, Mössbauer spectroscopy, and VT (19)F NMR spectroscopy. These complexes are part of a rare family of syn N-donor diiron(ii) compounds, [Fe2(X2PIM)(RCO2)2], that are structurally very similar to the active site of the hydroxylase enzyme component of reduced methane monooxygenase (MMOHred). Solution characterization of these complexes demonstrates that they undergo intramolecular carboxylate rearrangements, or carboxylate shifts, a dynamic feature relevant to the reactivity of the diiron centers in bacterial multicomponent monooxygenases.

摘要

一系列以氟原子作为核磁共振光谱探针的不对称羧酸桥联二价铁（II）配合物，即[Fe2(PIM)(Ar(4F-Ph)CO2)2]（10）、[Fe2(F2PIM)(Ar(Tol)CO2)2]（11）和[Fe2(F2PIM)(Ar(4F-Ph)CO2)2]（12），已通过X射线晶体学、穆斯堡尔光谱和变温（19）F核磁共振光谱进行了制备和表征。这些配合物是罕见的顺式N供体二价铁（II）化合物家族[Fe2(X2PIM)(RCO2)2]的一部分，其结构与还原型甲烷单加氧酶（MMOHred）的羟化酶酶组分的活性位点非常相似。对这些配合物的溶液表征表明，它们会发生分子内羧酸酯重排或羧酸酯迁移，这是一种与细菌多组分单加氧酶中二价铁中心反应性相关的动态特征。

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