An Artificial [Fe 4 S 4 ]-Containing Metalloenzyme for the Reduction of CO 2 to Hydrocarbons
Iron-sulfur clusters have been reported to catalyze various redox transformations, including the multielectron reduction of CO to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe S ]-containing Fischer-Tropschase relying on the biotin-streptavidin technology. For this pur...
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Veröffentlicht in: | Journal of the American Chemical Society 2023-07, Vol.145 (27), p.14823-14830 |
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creator | Waser, Valerie Mukherjee, Manjistha Tachibana, Ryo Igareta, Nico V Ward, Thomas R |
description | Iron-sulfur clusters have been reported to catalyze various redox transformations, including the multielectron reduction of CO
to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe
S
]-containing Fischer-Tropschase relying on the biotin-streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe
S
] 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
S
] cluster. The Fischer-Tropschase activity was improved by chemo-genetic means for the reduction of CO
to hydrocarbons with up to 14 turnovers. |
doi_str_mv | 10.1021/jacs.3c03546 |
format | Article |
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to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe
S
]-containing Fischer-Tropschase relying on the biotin-streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe
S
] 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
S
] cluster. The Fischer-Tropschase activity was improved by chemo-genetic means for the reduction of CO
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to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe
S
]-containing Fischer-Tropschase relying on the biotin-streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe
S
] 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
S
] cluster. The Fischer-Tropschase activity was improved by chemo-genetic means for the reduction of CO
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to hydrocarbons. Herein, we report the design and assembly of an artificial [Fe
S
]-containing Fischer-Tropschase relying on the biotin-streptavidin technology. For this purpose, we synthesized a bis-biotinylated [Fe
S
] 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
S
] cluster. The Fischer-Tropschase activity was improved by chemo-genetic means for the reduction of CO
to hydrocarbons with up to 14 turnovers.</abstract><cop>United States</cop><pmid>37387617</pmid><doi>10.1021/jacs.3c03546</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0001-6550-6262</orcidid><orcidid>https://orcid.org/0000-0001-8602-5468</orcidid><orcidid>https://orcid.org/0000-0002-1538-7266</orcidid></addata></record> |
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source | American Chemical Society Journals |
title | An Artificial [Fe 4 S 4 ]-Containing Metalloenzyme for the Reduction of CO 2 to Hydrocarbons |
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