Intercepting a transient non-hemic pyridine -oxide Fe() species involved in OAT reactions

In the context of bioinspired OAT catalysis, we developed a tetradentate dipyrrinpyridine ligand, a hybrid of hemic and non-hemic models. The catalytic activity of the iron( iii ) derivative was investigated in the presence of iodosylbenzene. Unexpectedly, MS, EPR, Mössbauer, UV-visible and FTIR spe...

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Published in:Chemical communications (Cambridge, England) England), 2021-11, Vol.57 (95), p.12836-12839
Main Authors: Vo, Nhat Tam, Herrero, Christian, Guillot, Régis, Inceoglu, Tanya, Leibl, Winfried, Clémancey, Martin, Dubourdeaux, Patrick, Blondin, Geneviève, Aukauloo, Ally, Sircoglou, Marie
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Summary:In the context of bioinspired OAT catalysis, we developed a tetradentate dipyrrinpyridine ligand, a hybrid of hemic and non-hemic models. The catalytic activity of the iron( iii ) derivative was investigated in the presence of iodosylbenzene. Unexpectedly, MS, EPR, Mössbauer, UV-visible and FTIR spectroscopic signatures supported by DFT calculations provide convincing evidence for the involvement of a relevant Fe III -O-N Py active intermediate. An unprecedented pyridine- N -oxide Fe( iii ) intermediate has been detected as a potent oxidizing species for catalytic OAT reactions.
ISSN:1359-7345
1364-548X
DOI:10.1039/d1cc04521k