An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons

[Image: see text] Iron–sulfur clusters have been reported to catalyze various redox transformations, including the multielectron reduction of CO(2) to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe(4)S(4)]-containing Fischer–Tropschase relying on the biotin–streptavidin...

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Autores principales: Waser, Valerie, Mukherjee, Manjistha, Tachibana, Ryo, Igareta, Nico V., Ward, Thomas R.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10347540/
https://www.ncbi.nlm.nih.gov/pubmed/37387617
http://dx.doi.org/10.1021/jacs.3c03546
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author Waser, Valerie
Mukherjee, Manjistha
Tachibana, Ryo
Igareta, Nico V.
Ward, Thomas R.
author_facet Waser, Valerie
Mukherjee, Manjistha
Tachibana, Ryo
Igareta, Nico V.
Ward, Thomas R.
author_sort Waser, Valerie
collection PubMed
description [Image: see text] Iron–sulfur clusters have been reported to catalyze various redox transformations, including the multielectron reduction of CO(2) to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe(4)S(4)]-containing Fischer–Tropschase relying on the biotin–streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe(4)S(4)] cofactor with marked aqueous stability and incorporated it in streptavidin. The effect of the second coordination sphere provided by the protein environment was scrutinized by cyclic voltammetry, highlighting the accessibility of the doubly reduced [Fe(4)S(4)] cluster. The Fischer–Tropschase activity was improved by chemo-genetic means for the reduction of CO(2) to hydrocarbons with up to 14 turnovers.
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spelling pubmed-103475402023-07-15 An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons Waser, Valerie Mukherjee, Manjistha Tachibana, Ryo Igareta, Nico V. Ward, Thomas R. J Am Chem Soc [Image: see text] Iron–sulfur clusters have been reported to catalyze various redox transformations, including the multielectron reduction of CO(2) to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe(4)S(4)]-containing Fischer–Tropschase relying on the biotin–streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe(4)S(4)] cofactor with marked aqueous stability and incorporated it in streptavidin. The effect of the second coordination sphere provided by the protein environment was scrutinized by cyclic voltammetry, highlighting the accessibility of the doubly reduced [Fe(4)S(4)] cluster. The Fischer–Tropschase activity was improved by chemo-genetic means for the reduction of CO(2) to hydrocarbons with up to 14 turnovers. American Chemical Society 2023-06-30 /pmc/articles/PMC10347540/ /pubmed/37387617 http://dx.doi.org/10.1021/jacs.3c03546 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Waser, Valerie
Mukherjee, Manjistha
Tachibana, Ryo
Igareta, Nico V.
Ward, Thomas R.
An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title_full An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title_fullStr An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title_full_unstemmed An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title_short An Artificial [Fe(4)S(4)]-Containing Metalloenzyme for the Reduction of CO(2) to Hydrocarbons
title_sort artificial [fe(4)s(4)]-containing metalloenzyme for the reduction of co(2) to hydrocarbons
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10347540/
https://www.ncbi.nlm.nih.gov/pubmed/37387617
http://dx.doi.org/10.1021/jacs.3c03546
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