Observation of Carbodicarbene Ligand Redox Noninnocence in Highly Oxidized Iron Complexes

Angewandte Chemie
Siu-Chung ChanJason England

Abstract

To probe the possibility that carbodicarbenes (CDCs) are redox active ligands, all four members of the redox series [Fe(1)2 ]n+ (n=2-5) were synthesized, where 1 is a neutral tridentate CDC. Through a combination of spectroscopy and DFT calculations, the electronic structure of the pentacation is shown to be [FeIII (1.+ )2 ]5+ (S= 1 / 2 ). That of [Fe(1)2 ]4+ is more ambiguous, but it has significant contributions from the open-shell singlet [FeIII (1)(1.+ )]4+ (S=0). The observed spin states derive from antiferromagnetic coupling of their constituent low-spin iron(III) centres and cation radical ligands. This marks the first time redox activity has been observed for carbones and expands the diverse chemical behaviour known for these ligands.

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Citations

Jan 27, 2019·Chemical Communications : Chem Comm·Jacob E WalleyRobert J Gilliard Jr
Feb 15, 2020·Chemical Science·Sebastian UllrichJörg Sundermeyer
May 1, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Sze-Wing NgChun-Yuen Wong
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Oct 30, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Lili ZhaoGernot Frenking
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Apr 30, 2021·Chemistry : a European Journal·Wei SuQing Ye
Apr 10, 2020·Inorganic Chemistry·Lisa GravoglKarsten Meyer
Feb 27, 2020·Inorganic Chemistry·Siu-Chung ChanJason England
Jun 14, 2019·Chemical Reviews·Marie Fustier-BoutignonNicolas Mézailles

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