Modular bimetallic complexes with a sulfonamido-based ligand†,Dalton Transactions

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Modular bimetallic complexes with a sulfonamido-based ligand†
Dalton Transactions ( IF 3.5 ) Pub Date : 2018-08-01 00:00:00 , DOI: 10.1039/c8dt02455c
Nathanael Lau ₁ , Yohei Sano , Joseph W Ziller , A S Borovik

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A series of bimetallic complexes prepared with the ligands N,N,N′,N′-tetramethylethane-1,2-diamine (TMEDA) and N,N′,N′′-[2,2′,2′′-nitrilotris(ethane-2,1-diyl)]tris(2,4,6-trimethylbenzenesulfonamido) ([MST]³⁻) is described. Four diiron compounds of the formulation (TMEDA)Fe^II(X)-(μ-OH)-Fe^IIIMST were prepared, in which the X⁻ ligands are the anions OTf⁻, Br⁻, SCN⁻, or N₃⁻. Additionally, two heterobimetallic compounds of the formulation (TMEDA)M^II(OTf)-(μ-OH)-Fe^IIIMST (M^II = Co^II or Ni^II) were synthesized. All these compounds have similar spectroscopic and structural properties. The diiron compounds exhibit perpendicular-mode electron paramagnetic resonance spectra consistent with S = 1/2 spin ground states, which is expected for high-spin Fe^II and Fe^III centres that are antiferromagnetically coupled. The heterobimetallic (TMEDA)Ni^II(OTf)-(μ-OH)-Fe^IIIMST complex had a spin state of S = 3/2 that also resulted from antiferromagnetic coupling between the high-spin Ni^II and Fe^III centres. The modularity of this system is further demonstrated by the substitution of the TMEDA ligand with ethylenediamine (en); for this species two equivalents of en coordinate to the Fe^II centre to form [(en)₂Fe^II-(μ-OH)-Fe^IIIMST]OTf. These results demonstrate that a modular bimetallic system has been developed in which the key components can be modified.

中文翻译：

具有磺酰胺基配体的模块化双金属配合物†

以配体N , N , N ', N '-四甲基乙烷-1,2-二胺 (TMEDA) 和N , N ', N ''-[2,2',2''-次氮基三酯制备的一系列双金属配合物描述了(乙烷-2,1-二基)]三(2,4,6-三甲基苯磺酰胺基)([MST] ^3- )。制备了配方为 (TMEDA)Fe ^II (X)-(μ-OH)-Fe ^III MST 的四种二铁化合物，其中 X ^-配体为阴离子 OTf ^- 、Br ^- 、SCN ^-或 N ₃ ^- 。此外，还合成了两种异双金属化合物（TMEDA）M ^II (OTf)-(μ-OH)-Fe ^III MST（M ^II = Co ^II或 Ni ^II ）。所有这些化合物都具有相似的光谱和结构特性。二铁化合物表现出与S = 1/2 自旋基态一致的垂直模式电子顺磁共振谱，这对于反铁磁耦合的高自旋 Fe ^II和 Fe ^III中心是预期的。异质双金属 (TMEDA)Ni ^II (OTf)-(μ-OH)-Fe ^III MST 复合物的自旋态为S = 3/2，这也是由高自旋 Ni ^II和 Fe ^III中心之间的反铁磁耦合产生的。通过用乙二胺 (en) 取代 TMEDA 配体进一步证明了该系统的模块化；对于该物种，两个当量的 en 与 Fe ^II中心配位形成 [(en) ₂ Fe ^II -(μ-OH)-Fe ^III MST]OTf。这些结果表明，已经开发出一种模块化双金属系统，其中的关键部件可以进行修改。

更新日期：2018-08-01

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