A DFT study on the C-H oxidation reactivity of Fe(iv)-oxo species with N4/N5 ligands derived from l-proline

利用密度泛函理论(DFT)研究了由L-脯氨酸衍生的N4/N5配体与Fe(IV)-氧代物种的CH氧化反应活性。

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Abstract

The hydroxylation of hexane by two Fe(IV)O complexes bearing a pentadentate ligand (N5, Pro3Py) and a tetradentate ligand (N4, Pro2PyBn) derived from l-proline was studied by DFT calculations. Theoretical results predict that both Fe(IV)O complexes hold triplet ground states. The hydrogen atom abstraction (HAA) processes by both Fe(IV)O species proceed through a two-state reactivity, thus indicating that HAA occurs via a low-barrier quintet surface. Beyond the conventional rebound step, the dissociation path is also calculated and is found to potentially occur after HAA.

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