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Final Stages in the Biosynthesis of the [FeFe]‐Hydrogenase Active Site.
- Source :
-
Angewandte Chemie International Edition . 5/27/2024, Vol. 63 Issue 22, p1-5. 5p. - Publication Year :
- 2024
-
Abstract
- The paper aims to elucidate the final stages in the biosynthesis of the [2Fe]H active site of the [FeFe]‐hydrogenases. The recently hypothesized intermediate [Fe2(SCH2NH2)2(CN)2(CO)4]2− ([1]2−) was prepared by a multistep route from [Fe2(S2)(CN)(CO)5]−. The following synthetic intermediates were characterized in order: [Fe2(SCH2NHFmoc)2(CNBEt3)(CO)5]−, [Fe2(SCH2NHFmoc)2(CN)−(CO)5]−, and [Fe2(SCH2NHFmoc)2(CN)2(CO)4]2−, where Fmoc is fluorenylmethoxycarbonyl). Derivatives of these anions include [K(18‐crown‐6)]+, PPh4+ and PPN+ salts as well as the 13CD2‐isotopologues. These Fe2 species exist as a mixture of two isomers attributed to diequatorial (ee) and axial‐equatorial (ae) stereochemistry at sulfur. In vitro experiments demonstrate that [1]2− maturates HydA1 in the presence of HydF and a cocktail of reagents. HydA1 can also be maturated using a highly simplified cocktail, omitting HydF and other proteins. This result is consistent with HydA1 participating in the maturation process and refines the roles of HydF. [ABSTRACT FROM AUTHOR]
- Subjects :
- *BIOSYNTHESIS
*STEREOCHEMISTRY
*SULFUR
*HYDROGENASE
*ANIONS
*ISOMERS
Subjects
Details
- Language :
- English
- ISSN :
- 14337851
- Volume :
- 63
- Issue :
- 22
- Database :
- Academic Search Index
- Journal :
- Angewandte Chemie International Edition
- Publication Type :
- Academic Journal
- Accession number :
- 177321202
- Full Text :
- https://doi.org/10.1002/anie.202404044