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EPR Spectroscopic Studies of [FeFe]-Hydrogenase Maturation.


ABSTRACT: Proton reduction and H2 oxidation are key elementary reactions for solar fuel production. Hydrogenases interconvert H+ and H2 with remarkable efficiency and have therefore received much attention in this context. For [FeFe]-hydrogenases, catalysis occurs at a unique cofactor called the H-cluster. In this article, we discuss ways in which EPR spectroscopy has elucidated aspects of the bioassembly of the H-cluster, with a focus on four case studies: EPR spectroscopic identification of a radical en route to the CO and CN- ligands of the H-cluster, tracing 57Fe from the maturase HydG into the H-cluster, characterization of the auxiliary Fe-S cluster in HydG, and isotopic labeling of the CN- ligands of HydA for electronic structure studies of its Hox state. Advances in cell-free maturation protocols have enabled several of these mechanistic studies, and understanding H-cluster maturation may in turn provide insights leading to improvements in hydrogenase production for biotechnological applications.

SUBMITTER: Suess DL 

PROVIDER: S-EPMC4618401 | biostudies-literature | 2015 Sep

REPOSITORIES: biostudies-literature

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EPR Spectroscopic Studies of [FeFe]-Hydrogenase Maturation.

Suess Daniel L M DL   Britt R David RD  

Catalysis letters 20150730 12


Proton reduction and H<sub>2</sub> oxidation are key elementary reactions for solar fuel production. Hydrogenases interconvert H<sup>+</sup> and H<sub>2</sub> with remarkable efficiency and have therefore received much attention in this context. For [FeFe]-hydrogenases, catalysis occurs at a unique cofactor called the H-cluster. In this article, we discuss ways in which EPR spectroscopy has elucidated aspects of the bioassembly of the H-cluster, with a focus on four case studies: EPR spectroscop  ...[more]

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