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Approche électrochimique de l'activation réductrice du dioxygène à l'aide d'un complexe de fer(II) non hémique

Abstract : Cytochrome P450 is a mononuclear iron enzyme, which catalyzes the oxidation of robust C-H bonds using O2. Activation of O2 is achieved at the Fe(II) center and requires an electron transfer to convert the iron(II)-dioxygen adduct into an iron(III)peroxo intermediate. After protonation, this latter may directly oxidize substrates or evolves to yield a powerful high valent iron-oxo moiety. In such natural systems, the necessary electrons are provided by a co-substrate NAD(P)H and are conveyed through a reductase.1The aim of this project is to develop non-heme iron(II) complexes as catalysts for the oxidation of small organic molecules by O2. Our objective is to use an electrode to deliver the electrons while providing mechanistic information at the same time thanks to a combined experimental/simulation approach using cyclic voltammetry. This work has shown that simple Fe(II) complexes bearing amine/pyridine ligands can activate O2 at an electrode surface following a mechanism that is reminiscent of the one of P450. However, the main scientific lock is to avoid the fast reduction of the reaction intermediates when they are generated at the electrode. We are currently studying how alterations of the first coordination sphere of the metal center and experimental conditions modulate the formation and the stability of these intermediates and thus, the efficiency of the catalysts.
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Submitted on : Wednesday, February 13, 2019 - 4:03:11 PM
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  • HAL Id : tel-02018125, version 1



Antoine Bohn. Approche électrochimique de l'activation réductrice du dioxygène à l'aide d'un complexe de fer(II) non hémique. Chimie analytique. Université Paris-Saclay, 2018. Français. ⟨NNT : 2018SACLS471⟩. ⟨tel-02018125⟩



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