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Redox Characterization of the Complex Molybdenum Enzyme Formate Dehydrogenase from Cupriavidus necator

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논문

Redox Characterization of the Complex Molybdenum Enzyme Formate Dehydrogenase from Cupriavidus necator

학술지

Journal of the American Chemical Society

저자명

Harmer, Jeffrey R.; Hakopian, Sheron; Niks, Dimitri; Hille, Russ; Bernhardt, Paul V.

초록

<P>The oxygen-tolerant and molybdenum-dependent formate dehydrogenase FdsDABG from <I>Cupriavidus necator</I> is capable of catalyzing both formate oxidation to CO<SUB>2</SUB> and the reverse reaction (CO<SUB>2</SUB> reduction to formate) at neutral pH, which are both reactions of great importance to energy production and carbon capture. FdsDABG is replete with redox cofactors comprising seven Fe/S clusters, flavin mononucleotide, and a molybdenum ion coordinated by two pyranopterin dithiolene ligands. The redox potentials of these centers are described herein and assigned to specific cofactors using combinations of potential-dependent continuous wave and pulse EPR spectroscopy and UV/visible spectroelectrochemistry on both the FdsDABG holoenzyme and the FdsBG subcomplex. These data represent the first redox characterization of a complex metal dependent formate dehydrogenase and provide an understanding of the highly efficient catalytic formate oxidation and CO<SUB>2</SUB> reduction activity that are associated with the enzyme.</P><BR>[FIG OMISSION]</BR>

발행연도

2023

발행기관

American Chemical Society

ISSN

0002-7863

ISSN

1520-5126

145

47

페이지

pp.25850-25863

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1 2023-12-11

논문; 2023-11-29

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