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Article Dans Une Revue Angewandte Chemie International Edition Année : 2017

A high‐valent non‐heme μ‐oxo manganese(IV) dimer generated from a thiolate‐bound manganese(II) complex and dioxygen

Résumé

This study deals with the unprecedented reactivity of dinuclear non-heme MnII -thiolate complexes with O2 , which dependent on the protonation state of the initial MnII dimer selectively generates either a di-μ-oxo or μ-oxo-μ-hydroxo MnIV complex. Both dimers have been characterized by different techniques including single-crystal X-ray diffraction and mass spectrometry. Oxygenation reactions carried out with labeled 18O2 unambiguously show that the oxygen atoms present in the MnIV dimers originate from O2 . Based on experimental observations and DFT calculations, evidence is provided that these MnIV species comproportionate with a MnIIprecursor to yield μ-oxo and/or μ-hydroxo MnIII dimers. Our work highlights the delicate balance of reaction conditions to control the synthesis of non-heme high-valent μ-oxo and μ-hydroxo Mn species from MnII precursors and O2 .
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Dates et versions

hal-02154187 , version 1 (15-12-2024)

Identifiants

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Déborah Brazzolotto, Fabián G. Cantú reinhard, Julian Smith-Jones, Marius Retegan, Lucia Amidani, et al.. A high‐valent non‐heme μ‐oxo manganese(IV) dimer generated from a thiolate‐bound manganese(II) complex and dioxygen. Angewandte Chemie International Edition, 2017, 56 (28), pp.8211-8215. ⟨10.1002/anie.201703215⟩. ⟨hal-02154187⟩
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