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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Unique mononuclear Mn-II complexes of an end-off compartmental Schiff base ligand: experimental and theoretical studies on their bio-relevant catalytic promiscuity
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Unique mononuclear Mn-II complexes of an end-off compartmental Schiff base ligand: experimental and theoretical studies on their bio-relevant catalytic promiscuity

机译：末端隔室席夫碱配体的独特单核Mn-II配合物：与生物相关的催化混杂的实验和理论研究

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摘要

Three new mononuclear manganese(II) complexes, namely [Mn(HL)(2)]center dot 2ClO(4) (1), [Mn(HL)(N(CN)(2)) (H2O)(2)]center dot ClO4 (2) and [Mn(HL)(SCN)(2)] (3) [LH = 4-tert-butyl-2,6-bis-[(2-pyridin-2-yl-ethylimino)-methyl]-phenol], have been synthesized and structurally characterized. An "end-off" compartmental ligand (LH) possesses two symmetrical compartments with N2O binding sites but accommodates only one manganese atom instead of two due to the protonation of the imine nitrogen of one compartment. Although all three complexes are mononuclear, complex 1 is unique as it has a 1 : 2 metal to ligand stoichiometry. The catalytic promiscuity of complexes 1-3 in terms of two different bio-relevant catalytic activities namely catecholase and phenoxazinone synthase has been thoroughly investigated. EPR and cyclic voltametric studies reveal that radical formation rather than metal centered redox participation is responsible for their catecholase-like and phenoxazinone synthase-like catalytic activity. A computational approach suggests that imine bond bound radical generation rather than phenoxo radical formation is most likely responsible for the oxidizing properties of the complexes.
机译：三种新的单核锰（II）配合物，即[Mn（HL）（2）]中心点2ClO（4）（1），[Mn（HL）（N（CN）（2））（H2O）（2）]中心点ClO4（2）和[Mn（HL）（SCN）（2）]（3）[LH = 4-叔丁基-2,6-双-[（2-吡啶-2-基-乙基亚氨基）-甲基]-苯酚]，已经合成并进行了结构表征。 “末端”隔室配体（LH）具有两个具有N2O结合位点的对称隔室，但由于一个隔室中亚胺氮的质子化，仅容纳一个锰原子而不是两个。尽管所有三个复合物都是单核的，但复合物1是独特的，因为它具有1：2的金属与配体化学计量比。就两种不同的生物相关催化活性（儿茶酚酶和苯恶嗪酮合酶）而言，对配合物1-3的催化混杂性进行了深入研究。 EPR和循环伏安研究表明，自由基形成而不是金属中心的氧化还原参与是其儿茶酚酶样和苯氧嗪酮合酶样催化活性的原因。一种计算方法表明，亚胺键结合的自由基的产生而不是苯氧自由基的形成最可能是造成复合物氧化性能的原因。

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