An Artificial Fe4S4-Containing Metalloenzyme for the Reduction of CO2 to Hydrocarbons

摘要

Iron-sulfurclusters have been reported to catalyzevariousredox transformations, including the multielectron reduction of CO2 to hydrocarbons. Herein, we report the design and assemblyof an artificial [Fe4S4]-containing Fischer-Tropschaserelying on the biotin-streptavidin technology. For this purpose,we synthesized a bis-biotinylated [Fe4S4] cofactorwith marked aqueous stability and incorporated it in streptavidin.The effect of the second coordination sphere provided by the proteinenvironment was scrutinized by cyclic voltammetry, highlighting theaccessibility of the doubly reduced [Fe4S4]cluster. The Fischer-Tropschase activity was improved by chemo-geneticmeans for the reduction of CO2 to hydrocarbons with upto 14 turnovers.