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本文引用的文献

1
Dioxygen Activation and Methane Hydroxylation by Soluble Methane Monooxygenase: A Tale of Two Irons and Three Proteins.可溶性甲烷单加氧酶对双原子氧的激活与甲烷羟基化作用：两个铁原子与三种蛋白质的故事
Angew Chem Int Ed Engl. 2001 Aug 3;40(15):2782-2807. doi: 10.1002/1521-3773(20010803)40:15<2782::AID-ANIE2782>3.0.CO;2-P.
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Phenoxyl radical complexes of gallium, scandium, iron and manganese.镓、钪、铁和锰的苯氧自由基配合物。
Chemistry. 1997 Feb;3(2):308-19. doi: 10.1002/chem.19970030221.
3
Correction. Assembly and characterization of an accurate model for the dron center in hemerythrin.更正。蚯蚓血红蛋白中dron中心精确模型的组装与表征。
J Am Chem Soc. 1986 Feb 1;108(3):557. doi: 10.1021/ja00263a600.
4
Heterolytic dissociation of water demonstrated by crystal-to-crystal core interconversion from (μ-oxo)divanadium to bis(μ-hydroxo)divanadium substituted polyoxometalates.通过（μ-氧代）钒到双（μ-羟）取代多金属氧酸盐的晶体-晶体核相互转化证明水的异裂离解。
J Am Chem Soc. 2011 Feb 16;133(6):1622-5. doi: 10.1021/ja108245g. Epub 2011 Jan 7.
5
The aging-associated enzyme CLK-1 is a member of the carboxylate-bridged diiron family of proteins.衰老相关酶 CLK-1 是羧酸桥联双核铁蛋白家族的成员。
Biochemistry. 2010 Nov 16;49(45):9679-81. doi: 10.1021/bi101475z. Epub 2010 Oct 21.
6
Current challenges of modeling diiron enzyme active sites for dioxygen activation by biomimetic synthetic complexes.当前模拟双铁酶活性位点用于生物模拟合成配合物激活氧气的挑战。
Chem Soc Rev. 2010 Aug;39(8):2768-79. doi: 10.1039/c003079c. Epub 2010 May 20.
7
Just a proton: distinguishing the two electronic states of five-coordinate high-spin iron(II) porphyrinates with imidazole/ate coordination.仅有一个质子：通过咪唑/酸配位区分五配位高自旋亚铁(II)卟啉的两种电子态。
J Am Chem Soc. 2010 Mar 24;132(11):3737-50. doi: 10.1021/ja907584x.
8
2-Phenoxypyridyl dinucleating ligands for assembly of diiron(II) complexes: efficient reactivity with O(2) to form (mu-Oxo)diiron(III) units.2-苯氧基吡啶双齿配体用于二铁(II)配合物的组装：与 O(2)的高效反应性形成（μ-氧代）二铁(III)单元。
Inorg Chem. 2009 Nov 16;48(22):10708-19. doi: 10.1021/ic901711c.
9
Low-molecular-weight analogues of the soluble methane monooxygenase (sMMO): from the structural mimicking of resting states and intermediates to functional models.可溶性甲烷单加氧酶（sMMO）的低分子量类似物：从静止状态和中间体的结构模拟到功能模型
Chemistry. 2009 Oct 12;15(40):10316-28. doi: 10.1002/chem.200901910.
10
Human deoxyhypusine hydroxylase, an enzyme involved in regulating cell growth, activates O2 with a nonheme diiron center.人类脱氧hypusine羟化酶是一种参与调节细胞生长的酶，它通过一个非血红素双铁中心激活氧气。
Proc Natl Acad Sci U S A. 2009 Sep 1;106(35):14814-9. doi: 10.1073/pnas.0904553106. Epub 2009 Aug 19.

朝向功能化的羧酸桥联双核铁蛋白模拟物：使用大环配体框架实现结构稳定性和构象灵活性。

Toward functional carboxylate-bridged diiron protein mimics: achieving structural stability and conformational flexibility using a macrocylic ligand framework.

机构信息

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

出版信息

J Am Chem Soc. 2011 Jul 13;133(27):10568-81. doi: 10.1021/ja2021312. Epub 2011 Jun 17.

DOI:10.1021/ja2021312
PMID:21682286
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC3149837/
Abstract

A dinucleating macrocycle, H(2)PIM, containing phenoxylimine metal-binding units has been prepared. Reaction of H(2)PIM with [Fe(2)(Mes)(4)] (Mes = 2,4,6-trimethylphenyl) and sterically hindered carboxylic acids, Ph(3)CCO(2)H or Ar(Tol)CO(2)H (2,6-bis(p-tolyl)benzoic acid), afforded complexes [Fe(2)(PIM)(Ph(3)CCO(2))(2)] (1) and [Fe(2)(PIM)(Ar(Tol)CO(2))(2)] (2), respectively. X-ray diffraction studies revealed that these diiron(II) complexes closely mimic the active site structures of the hydroxylase components of bacterial multicomponent monooxygenases (BMMs), particularly the syn disposition of the nitrogen donor atoms and the bridging μ-η(1)η(2) and μ-η(1)η(1) modes of the carboxylate ligands at the diiron(II) centers. Cyclic voltammograms of 1 and 2 displayed quasi-reversible redox couples at +16 and +108 mV vs ferrocene/ferrocenium, respectively. Treatment of 2 with silver perchlorate afforded a silver(I)/iron(III) heterodimetallic complex, [Fe(2)(μ-OH)(2)(ClO(4))(2)(PIM)(Ar(Tol)CO(2))Ag] (3), which was structurally and spectroscopically characterized. Complexes 1 and 2 both react rapidly with dioxygen. Oxygenation of 1 afforded a (μ-hydroxo)diiron(III) complex [Fe(2)(μ-OH)(PIM)(Ph(3)CCO(2))(3)] (4), a hexa(μ-hydroxo)tetrairon(III) complex [Fe(4)(μ-OH)(6)(PIM)(2)(Ph(3)CCO(2))(2)] (5), and an unidentified iron(III) species. Oxygenation of 2 exclusively formed di(carboxylato)diiron(III) compounds, a testimony to the role of the macrocylic ligand in preserving the dinuclear iron center under oxidizing conditions. X-ray crystallographic and (57)Fe Mössbauer spectroscopic investigations indicated that 2 reacts with dioxygen to give a mixture of (μ-oxo)diiron(III) [Fe(2)(μ-O)(PIM)(Ar(Tol)CO(2))(2)] (6) and di(μ-hydroxo)diiron(III) [Fe(2)(μ-OH)(2)(PIM)(Ar(Tol)CO(2))(2)] (7) units in the same crystal lattice. Compounds 6 and 7 spontaneously convert to a tetrairon(III) complex, [Fe(4)(μ-OH)(6)(PIM)(2)(Ar(Tol)CO(2))(2)] (8), when treated with excess H(2)O.

摘要

一种双氮大环化合物 H(2)PIM，其中包含苯并恶嗪金属结合单元，已经被制备出来。H(2)PIM 与 [Fe(2)(Mes)(4)]（Mes = 2,4,6-三甲基苯基）和空间位阻羧酸 Ph(3)CCO(2)H 或 Ar(Tol)CO(2)H（2,6-双（对甲苯基）苯甲酸）反应，分别得到了配合物 [Fe(2)(PIM)(Ph(3)CCO(2))(2)]（1）和 [Fe(2)(PIM)(Ar(Tol)CO(2))(2)]（2）。X 射线衍射研究表明，这些二铁(II)配合物紧密模拟了细菌多组分单加氧酶（BMM）中羟化酶成分的活性部位结构，特别是氮供体原子的顺式排列以及羧酸盐配体在二铁(II)中心的桥联 μ-η(1)η(2)和 μ-η(1)η(1)模式。1 和 2 的循环伏安图在+16 和+108 mV 相对于铁电/铁电对分别显示出准可逆氧化还原对。2 与高氯酸银反应得到了银(I)/铁(III)杂二金属配合物 [Fe(2)(μ-OH)(2)(ClO(4))(2)(PIM)(Ar(Tol)CO(2))Ag]（3），其结构和光谱特征已得到证实。配合物 1 和 2 均能快速与氧气反应。1 的氧合作用生成了（μ-羟基金属）二铁(III)配合物 [Fe(2)(μ-OH)(PIM)(Ph(3)CCO(2))(3)]（4）、六（μ-羟基金属）四铁(III)配合物 [Fe(4)(μ-OH)(6)(PIM)(2)(Ph(3)CCO(2))(2)]（5）和一种未鉴定的铁(III)物种。2 的氧合作用仅形成二（羧酸盐）二铁(III)化合物，这证明了大环配体在氧化条件下保持双核铁中心的作用。X 射线晶体学和 (57)Fe Mössbauer 光谱研究表明，2 与氧气反应生成（μ-氧基金属）二铁(III) [Fe(2)(μ-O)(PIM)(Ar(Tol)CO(2))(2)]（6）和二（μ-羟基金属）二铁(III) [Fe(2)(μ-OH)(2)(PIM)(Ar(Tol)CO(2))(2)]（7）在同一晶体晶格中的混合物。当用过量的 H(2)O 处理时，化合物 6 和 7 会自发转化为四铁(III)配合物 [Fe(4)(μ-OH)(6)(PIM)(2)(Ar(Tol)CO(2))(2)]（8）。