A terminal FeOH complex, [Fe(L)(OH)] (), has been synthesized and structurally characterized (HL = 1,2-bis(2-hydroxy-2-methylpropanamido)benzene). The oxidation reaction of with one equiv. of (4-bromophenyl)ammoniumyl hexachloroantimonate (TBAH) or ceric ammonium nitrate (CAN) in acetonitrile at -45 °C results in the formation of a FeOH ligand radical complex, [Fe(L˙)(OH)] (), which is hereby characterized by UV-visible, H nuclear magnetic resonance, electron paramagnetic resonance, and X-ray absorption spectroscopy techniques. The reaction of with a triphenylcarbon radical further gives triphenylmethanol and mimics the so-called oxygen rebound step of Cpd II of cytochrome P450. Furthermore, the reaction of was explored with different 4-substituted-2,6-di--butylphenols. Based on kinetic analysis, a hydrogen atom transfer (HAT) mechanism has been established. A p value of 19.3 and a BDFE value of 78.2 kcal/mol have been estimated for complex .
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| http://dx.doi.org/10.1039/d0sc07054h | DOI Listing |
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