A Synthetic Model of Enzymatic [Fe4 S4 ]-Alkyl Intermediates

Journal of the American Chemical Society
Mengshan YeDaniel L M Suess

Abstract

Although alkyl complexes of [Fe4S4] 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 [Fe4S4]2+-alkyl cluster. Whereas [Fe4S4]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 [Fe4S4] clusters.

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Citations

Aug 25, 2020·Chemical Communications : Chem Comm·Manar M Shoshani, Theodor Agapie
Jan 15, 2021·Inorganic Chemistry·Amy L SpeelmanPatrick L Holland
May 28, 2020·Chemical Reviews·Kazuki Tanifuji, Yasuhiro Ohki
Jul 23, 2020·Journal of the American Chemical Society·Alexandra C Brown, Daniel L M Suess
Sep 26, 2020·Journal of the American Chemical Society·Charles H ArnettTheodor Agapie
Mar 28, 2021·Angewandte Chemie·Arun SridharanDaniel L M Suess
Jul 22, 2020·Journal of the American Chemical Society·Alex McSkimmingDaniel L M Suess
Jun 8, 2021·Chemical Science·Alexandra L NagelskiPatrick L Holland
Jun 24, 2021·Chemical Society Reviews·Chen-Hao Wang, Serena DeBeer
Apr 24, 2020·Inorganic Chemistry·Stefanie DehnenWilliam B Tolman
Nov 14, 2020·ACS Synthetic Biology·Bhanu P JagilinkiVikas Nanda
Dec 4, 2021·Proceedings of the National Academy of Sciences of the United States of America·Linh N V LeTheodor Agapie

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Methods Mentioned

BETA
X-ray

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