Flash Communication: Flexibility of a Biologically Inspired Ligand Framework for Intramolecular C-H Activation

快讯:生物启发式配体框架在分子内CH活化中的灵活性

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Abstract

High-valent iron complexes play a crucial role in the oxidation of organic substrates, especially in C-H bond functionalization reactions in biology. This paper investigates the reactivity of nonporphyrin tripodal ligands featuring a secondary coordination sphere, focusing on their prospective ability to stabilize high-valent iron-oxo species. Using NMR spectroscopy and X-ray crystallography, we detail the formation of an Fe(III)-alkoxide complex through intramolecular C-H bond activation, providing insight into the potential transient formation of a high-valent iron-oxo intermediate. While attempts to observe an Fe(IV)-oxo complex were unsuccessful, our findings underscore the significance of the ligand electronic environment in stabilizing reactive iron species for C-H bond activation.

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