Journal
INORGANIC CHEMISTRY
Volume 48, Issue 21, Pages 10036-10048Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic9005086
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- Australian Research Council
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The binuclear heterovalent manganese model complex [Mn(II)Mn(III)(L1)(OAc2] ClO4 center dot H2O (H(2)L1 = 2-(((3-((bis(pyridin-2-ylmethyl)amino)methyl)-2-hydroxy-5-methylbenzyl)(pyridin-2-ylmethyl)amino)-methyl)phenol) has been prepared and studied structurally, spectroscopically, and computationally. The magnetic and electronic properties of the complex have been related to its structure. The complex is weakly antiferromagnetically coupled (J similar to -5 cm 1, H = -2J S-1 center dot S-2) and the electron paramagnetic resonance (EPR) and magnetic circular dichroism (MCD) spectra identify the Jahn-Teller distortion of the Mn(III) center as predominantly a tetragonal compression, with a significant rhombic component. Electronic structure calculations using density functional theory have confirmed the conclusions derived from the experimental investigations. In contrast to isostructural M(II)Fe(III) complexes (M = Fe, Mn, Zn, Ni), the Mn(II)Mn(III) system is bifunctional possessing both catalase and hydrolase activities, and only one catalytically relevant pK(a) (= 8.2) is detected. Mechanistic implications are discussed.
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