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9-三联苯羧酸桥联二铁（II）配合物：桨轮几何异构体的捕获

9-Triptycenecarboxylate-Bridged Diiron(II) Complexes: Capture of the Paddlewheel Geometric Isomer.

作者信息

Friedle Simone, Kodanko Jeremy J, Fornace Kyrstin L, Lippard Stephen J

机构信息

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

出版信息

J Mol Struct. 2008 Nov 12;890(1-3):317-327. doi: 10.1016/j.molstruc.2008.05.030.

DOI:10.1016/j.molstruc.2008.05.030
PMID:19915653
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC2610540/
Abstract

The synthesis and characterization of diiron(II) complexes supported by 9-triptycenecarboxylate ligands ((-)O(2)CTrp) is described. The interlocking nature of the triptycenecarboxylates facilitates formation of quadruply bridged diiron(II) complexes of the type [Fe(2)(μ-O(2)CTrp)(4)(L)(2)] (L = THF, pyridine or imidazole derivative) with a paddlewheel geometry. A systematic lengthening of the Fe-Fe distance occurs with the increase in steric bulk of the neutral donor L, resulting in values of up to 3 Å without disassembly of the paddlewheel structure. Reactions with an excess of water do not lead to decomposition of the diiron(II) core, indicating that these quadruply bridged complexes are of exceptional stability. The red-colored complexes [Fe(2)(μ-O(2)CTrp)(4)(4-AcPy)(2)] (10) and [Fe(2)(μ-O(2)CTrp)(4)(4-CNPy)(2)] (11) exhibit solvent-dependent thermochromism in coordinating solvents that was studied by variable temperature UV-vis spectroscopy. Reaction of [Fe(2)(μ-O(2)CTrp)(4)(THF)(2)] with N,N,N',N'-tetramethylethylenediamine (TMEDA), tetra-n-butyl ammonium thiocyanate, or excess 2-methylimidazole resulted in the formation of mononuclear complexes [Fe(O(2)CTrp)(2)(TMEDA)] (13), (n-Bu(4)N)(2)[Fe(O(2)CTrp)(2)(SCN)(2)] (14), and [Fe(O(2)CTrp)(2)(2-MeIm)(2)] (15) having an O(4)/N(2) coordination sphere composition.

摘要

描述了由9-三蝶烯羧酸酯配体((-)O₂CTrp)支撑的二铁(II)配合物的合成与表征。三蝶烯羧酸盐的互锁性质有利于形成具有桨轮几何结构的[Fe₂(μ-O₂CTrp)₄(L)₂]型四重桥连二铁(II)配合物（L = 四氢呋喃、吡啶或咪唑衍生物）。随着中性供体L空间位阻的增加，Fe-Fe距离会系统性地变长，在桨轮结构不拆解的情况下，Fe-Fe距离可达3 Å。与过量水的反应不会导致二铁(II)核的分解，这表明这些四重桥连配合物具有非凡的稳定性。红色配合物[Fe₂(μ-O₂CTrp)₄(4-AcPy)₂] (10)和[Fe₂(μ-O₂CTrp)₄(4-CNPy)₂] (11)在配位溶剂中表现出溶剂依赖性热致变色，通过变温紫外-可见光谱对其进行了研究。[Fe₂(μ-O₂CTrp)₄(THF)₂]与N,N,N',N'-四甲基乙二胺(TMEDA)、四正丁基硫氰酸铵或过量的2-甲基咪唑反应，生成了具有O₄/N₂配位球组成的单核配合物[Fe(O₂CTrp)₂(TMEDA)] (13)、(n-Bu₄N)₂[Fe(O₂CTrp)₂(SCN)₂] (14)和[Fe(O₂CTrp)₂(2-MeIm)₂] (15)。

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本文引用的文献

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A Bulky Benzoate Ligand for Modeling the Carboxylate-Rich Active Sites of Non-Heme Diiron Enzymes.一种用于模拟非血红素二铁酶富含羧酸盐活性位点的庞大苯甲酸酯配体。
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