A Molecular Low-Coordinate [Fe-S-Fe] Unit in Three Oxidation States

Chemistry. 2021 Apr 7;27(20):6348-6353. doi: 10.1002/chem.202100336. Epub 2021 Mar 5.

Abstract

A [Fe-S-Fe] subunit with a single sulfide bridging two low-coordinate iron ions is the supposed active site of the iron-molybdenum co-factor (FeMoco) of nitrogenase. Here we report a dinuclear monosulfido bridged diiron(II) complex with a similar complex geometry that can be oxidized stepwise to diiron(II/III) and diiron(III/III) complexes while retaining the [Fe-S-Fe] core. The series of complexes has been characterized crystallographically, and electronic structures have been studied using, inter alia, 57 Fe Mössbauer spectroscopy and SQUID magnetometry. Further, cleavage of the [Fe-S-Fe] unit by CS2 is presented.

Keywords: 57Fe Mössbauer spectroscopy; electrochemistry; iron sulfide complex; magnetism; nitrogenase.