4.7 Article

Triiron clusters derived from dinuclear complexes related to the active site of [Fe-Fe] hydrogenases: steric effect of the dithiolate bridge on redox properties, a DFT analysis

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INORGANIC CHEMISTRY FRONTIERS
卷 8, 期 15, 页码 3659-+

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d1qi00006c

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The synthesis, structural characterization, and electrochemical properties of triiron clusters with different dithiolate bridges were studied, focusing on their protonation and redox behaviors. The impact of the dithiolate bridges on the complexes' electrochemical properties was investigated using cyclic voltammetry and DFT calculations.
A series of triiron clusters [Fe-dppe)(mu-pdt)(mu-pdt)] featuring different combinations of dithiolate bridges have been prepared by using dinuclear and mononuclear precursors, [Fe(mu-xdt)] (xdt = pdt, pdt, pdt, adt) and [Fe(CO)>-dppe)(kappa(2)-pdt)]. Novel triiron compounds, featuring sterically crowded dithiolate bridges (pdt, pdt), were spectroscopically and structurally characterized. Their protonation and redox behaviours are discussed. The effect of the dithiolate bridges on the electrochemical properties (oxidation and reduction) of the complexes [Fe(CO)dppe)(mu-xdt)(mu-pdt)] has been examined by cyclic voltammetry and rationalized by DFT calculations. Studies on the protonation of these species and their proton reduction behaviour were considered.

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