Observation of Radical Rebound in a Mononuclear Nonheme Iron Model Complex,Journal of the American Chemical Society

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Observation of Radical Rebound in a Mononuclear Nonheme Iron Model Complex
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-03-14 , DOI: 10.1021/jacs.7b12707
Thomas M Pangia ₁ , Casey G Davies ₂ , Joshua R Prendergast _{2,

3} , Jesse B Gordon ₁ , Maxime A Siegler ₁ , Guy N L Jameson _{2,

3} , David P Goldberg ₁

Affiliation

A nonheme iron(III) terminal methoxide complex, [FeIII(N3PyO2Ph)(OCH3)]ClO4, was synthesized. Reaction of this complex with the triphenylmethyl radical (Ph3C•) leads to formation of Ph3COCH3 and the one-electron-reduced iron(II) center, as seen by UV-vis, EPR, 1H NMR, and Mössbauer spectroscopy. These results indicate that homolytic Fe-O bond cleavage occurs together with C-O bond formation, providing a direct observation of the "radical rebound" process proposed for both biological and synthetic nonheme iron centers.

中文翻译：

单核非血红素铁模型复合物中自由基反弹的观察

合成了非血红素铁(III)末端甲醇复合物[FeIII(N3PyO2Ph)(OCH3)]ClO4。该配合物与三苯甲基自由基 (Ph3C•) 的反应导致形成 Ph3COCH3 和单电子还原铁 (II) 中心，如 UV-vis、EPR、1H NMR 和穆斯堡尔光谱所示。这些结果表明，均裂 Fe-O 键断裂与 CO 键形成同时发生，提供了对生物和合成非血红素铁中心提出的“自由基反弹”过程的直接观察。

更新日期：2018-03-14

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