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Although alkyl complexes of [Fe 4 S 4 ] clusters have been invoked as intermediates in a number of enzymatic reactions, obtaining a detailed understanding of their reactivity patterns and electronic structures has been difficult owing to their transient nature. To address this challenge, we herein report the synthesis and characterization of a 3:1 site-differentiated [Fe 4 S 4 ] 2+ -alkyl cluster. Whereas [Fe 4 S 4 ] 2+ clusters typically exhibit pairwise delocalized electronic structures in which each Fe has a formal valence of 2.5+, Mössbauer spectroscopic and computational studies suggest that the highly electron-releasing alkyl group partially localizes the charge distribution within the cubane, an effect that has not been previously observed in tetrahedrally coordinated [Fe 4 S 4 ] clusters.

A Synthetic Model of Enzymatic [Fe4S4]–Alkyl Intermediates

A Synthetic Model of Enzymatic [Fe₄S₄]–Alkyl Intermediates