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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >New cyanide-bridged Mn~(III)-M~(III) heterometallic dinuclear complexes constructed from [M~(III)(AA)(CN)_4] ~- building blocks (M = Cr and Fe): Synthesis, crystal structures and magnetic properties
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New cyanide-bridged Mn~(III)-M~(III) heterometallic dinuclear complexes constructed from [M~(III)(AA)(CN)_4] ~- building blocks (M = Cr and Fe): Synthesis, crystal structures and magnetic properties

机译：[[M〜（III）（AA）（CN）_4]〜-（M = Cr and Fe）构成的新型氰化物桥联的Mn〜（III）-M〜（III）杂金属双核配合物：合成，晶体结构和磁性

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摘要

Three Mn~(III)-M~(III) (M = Cr and Fe) dinuclear complexes have been obtained by assembling [Mn~(III)(SB)(H_2O)] ~+ and [M~(III)(AA)(CN)_4]~- ions, where SB is the dianion of the Schiff-base resulting from the condensation of 3-methoxysalicylaldehyde with ethylenediamine (3-MeOsalen~(2-)) or 1,2-cyclohexanediamine (3-MeOsalcyen~(2-)): [Mn(3-MeOsalen)(H _2O)(-NC)Cr(bipy)(CN)_3]·2H_2O (1), [Mn(3-MeOsalen)(H_2O)(-NC)Cr(ampy)(CN)_3][Mn(3-MeOsalen) (H_2O)_2]ClO4·2H_2O (2) and [Mn(3-MeOsalcyen)(H_2O)(-NC)Fe(bpym)(CN)_3]·3H _2O (3) (bipy = 2,2′-bipyridine, ampy = 2-aminomethylpyridine and bpym = 2,2′-bipyrimidine). The [M(AA)(CN)4]- unit in 1-3 acts as a monodentate ligand towards the manganese(iii) ion through one of its four cyanide groups. The manganese(iii) ion in 1-3 exhibits an elongated octahedral stereochemistry with the tetradentate SB building the equatorial plane and a water molecule and a cyanide-nitrogen atom filling the axial positions. Remarkably, the neutral mononuclear complex [Mn(3-MeOsalen)(H_2O)_2]ClO_4 co-crystallizes with the heterobimetallic unit in 2. The values of the Mn~(III)-M ~(III) distance across the bridging cyanide are 5.228 (1), 5.505 (2) and 5.265 ? (3). The packing of the neutral heterobimetallic units in the crystal is governed by the self-complementarity of the [Mn(SB)(H _2O)]~+ moieties, which interact each other through hydrogen bonds established between the aqua ligand from one fragment with the set of phenolate- and methoxy-oxygens from the adjacent one. The magnetic properties of the three complexes have been investigated in the temperature range 1.9-300 K. Weak antiferromagnetic interactions between the Mn~(III) and M ~(III) ions across the cyanido bridge were found: JMnM = -5.6 (1), -0.63 (2) and -2.4 cm-1 (3) the Hamiltonian being defined as H = -JSMn·SM. Theoretical calculations based on density functional theory (DFT) have been used to substantiate both the nature and magnitude of the exchange interactions observed and also to analyze the dependence of the magnetic coupling on the structural parameters within the Mn~(III)-N-C-M~(III) motif in 1-3.
机译：通过组装[Mn〜（III）（SB）（H_2O）]〜+和[M〜（III）（AA）（AA）获得了三种Mn（III）-M（III）（M = Cr和Fe）双核配合物）（CN）_4]-离子，其中SB是3-甲氧基水杨醛与乙二胺（3-MeOsalen〜（2-））或1,2-环己二胺（3-MeOsalcyen）缩合形成的席夫碱的二价阴离子〜（2-））：[Mn（3-MeOsalen）（H _2O）（-NC）Cr（bipy）（CN）_3]·2H_2O（1），[Mn（3-MeOsalen）（H_2O）（-NC ）Cr（ampy）（CN）_3] [Mn（3-MeOsalen）（H_2O）_2] ClO4·2H_2O（2）和[Mn（3-MeOsalcyen）（H_2O）（-NC）Fe（bpym）（CN） _3]·3H _2O（3）（bipy = 2,2'-联吡啶，ampy = 2-氨基甲基吡啶和bpym = 2,2'-联嘧啶）。 1-3中的[M（AA）（CN）4]-单元通过其四个氰化物基团之一充当锰（iii）离子的单齿配体。 1-3中的锰（iii）离子具有细长的八面体立体化学结构，四齿SB构成赤道平面，水分子和氰化物-氮原子填充轴向位置。值得注意的是，中性单核络合物[Mn（3-MeOsalen）（H_2O）_2] ClO_4与杂双金属单元在2中共结晶。跨桥氰化物的Mn〜（III）-M〜（III）距离的值为5.228（1），5.505（2）和5.265？ （3）。晶体中中性异双金属单元的堆积受[Mn（SB）（H _2O）]〜+部分的自互补性支配，后者通过一个片段的水配体与氢键之间建立的氢键相互作用。相邻的一组酚盐和甲氧基。在1.9-300 K的温度范围内研究了这三种配合物的磁性。发现氰基桥上的Mn〜（III）和M〜（III）离子之间弱的反铁磁相互作用：JMnM = -5.6（1） ，-0.63（2）和-2.4 cm-1（3）哈密顿量定义为H = -JSMn·SM。基于密度泛函理论（DFT）的理论计算已被用来证实所观察到的交换相互作用的性质和大小，并用于分析磁耦合对Mn〜（III）-NCM〜（ III）1-3中的主题。

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