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首页> 外文期刊>Polyhedron: The International Journal for Inorganic and Organometallic Chemistry >Compartmental unsymmetrical lateral macrobicyclic ligands with an aromatic backbone providing a phenoxo bridge: synthetic, spectral, magnetic, electrochemical and kinetic features of mono and binuclear copper(II) complexes
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Compartmental unsymmetrical lateral macrobicyclic ligands with an aromatic backbone providing a phenoxo bridge: synthetic, spectral, magnetic, electrochemical and kinetic features of mono and binuclear copper(II) complexes

机译：具有芳香族骨架的隔室不对称侧向大环双环配体，形成苯氧桥：单核和双核铜（II）配合物的合成，光谱，磁性，电化学和动力学特征

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摘要

From macrobicyclic ligands having different compartments originated from their corresponding precursor compounds (PC-1: 3,4:9,10-dibenzo-1,12[N,N'-bis{(3-formyl-2-hydroxy-5-methyl)benzyl}diaza]-5,8-dioxacyclotetradecane and PC-2: 3,4:9,10-dibenzo-1,12[N,N'-bis{(3-formyl-2-hydroxy-5-methyl)benzyl}diaza]-5,8-dioxacyclopentadecane) several mono and binuclear copper(H) complexes denoted as [CuL](ClO)(4) and [Cu2L(ClO4)](ClO4) have been synthesized. Electrochemical studies vindicate that one quasireversible reduction wave (E-pc = -0.80 to -0.88 V) for the mononuclear complexes and two quasireversible one electron transfer reduction waves (E-pc(1) = -0.84 to -0.94 V, E-pc(2) = - 1.25 to - 1.40 V) for the binuclear complexes are obtained in the cathodic region. The probe of room temperature magnetic moment studies depicts the presence of an antiferromagnetic interaction in the binuclear complexes (mu(eff) of 1.35-1.42 B.M.), which is also observed from the broad ESR spectra with a g value of 2.10 or 2.11. Whereas, hyperfine splitting in ESR spectra is observed for mononuclear complexes and the magnetic moment value is found to be close to the spin only value (mu(eff) of 1.69-1.71 B.M.). A variable temperature magnetic susceptibility study of the complex was carried out and the calculated -2J values for the binuclear complexes [Cu2L1a (ClO4)](ClO4) and [Cu2L1b (ClO4)](ClO4) are 240 and 219 cm(-1), respectively. The initial rate constant values of catechol oxidation using the complexes as catalysts have been found to span a domain ranging from 5.06 x 10(-3) to 2.56 x 10(-2) min(-1) and the values are found to be higher for binuclear complexes than the corresponding mononuclear complexes. Spectral, electrochemical and catalytic studies support the distortion of the copper ion geometry that arises as the macrocyclic ring size increases. (C) 2003 Elsevier Ltd. All rights reserved.
机译：来自具有不同区室的大双环配体，源自其相应的前体化合物（PC-1：3,4：9,10-二苯并-1,12 [N，N'-双{（3-甲酰基-2-羟基-5-甲基）苄基}二氮杂] -5,8-二氧杂环十四烷和PC-2：3,4：9,10-二苯并-1,12 [N，N'-双{（3-甲酰基-2-羟基-5-甲基）合成了[CuL]（ClO）（4）和[Cu2L（ClO4）]（ClO4）表示的几种单核和双核铜（H）配合物。电化学研究证明，单核络合物有一个准可逆还原波（E-pc = -0.80至-0.88 V），两个准拟可逆还原波（E-pc（1）= -0.84至-0.94 V，E-pc （2）=-1.25至-1.40 V），在阴极区域获得双核配合物。室温磁矩研究的探针描述了在双核络合物中存在反铁磁相互作用（mu（eff）为1.35-1.42 B.M.），这也从g值为2.10或2.11的宽ESR光谱中观察到。然而，对于单核络合物，在ESR谱中观察到超细分裂，并且发现磁矩值接近仅自旋值（μ（eff）为1.69-1.71B.M。）。对该化合物进行了可变温度磁化率研究，计算出的双核配合物[Cu2L1a（ClO4）]（ClO4）和[Cu2L1b（ClO4）]（ClO4）的-2J值为240和219 cm（-1） ， 分别。已发现使用络合物作为催化剂的邻苯二酚氧化的初始速率常数值范围介于5.06 x 10（-3）到2.56 x 10（-2）min（-1）之间，并且发现该值更高双核复合物比相应的单核复合物大。光谱，电化学和催化研究都支持随着大环尺寸的增加而引起的铜离子几何形状的畸变。 （C）2003 Elsevier Ltd.保留所有权利。

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