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TitleStructure and electron transfer pathways of an electron-bifurcating NiFe-hydrogenase.
Journal, issue, pagesSci Adv, Vol. 8, Issue 8, Page eabm7546, Year 2022
Publish dateFeb 25, 2022
AuthorsXiang Feng / Gerrit J Schut / Dominik K Haja / Michael W W Adams / Huilin Li /
PubMed AbstractElectron bifurcation enables thermodynamically unfavorable biochemical reactions. Four groups of bifurcating flavoenzyme are known and three use FAD to bifurcate. FeFe-HydABC hydrogenase represents ...Electron bifurcation enables thermodynamically unfavorable biochemical reactions. Four groups of bifurcating flavoenzyme are known and three use FAD to bifurcate. FeFe-HydABC hydrogenase represents the fourth group, but its bifurcation site is unknown. We report cryo-EM structures of the related NiFe-HydABCSL hydrogenase that reversibly oxidizes H and couples endergonic reduction of ferredoxin with exergonic reduction of NAD. FMN surrounded by a unique arrangement of iron sulfur clusters forms the bifurcating center. NAD binds to FMN in HydB, and electrons from H via HydA to a HydB [4Fe-4S] cluster enable the FMN to reduce NAD. Low-potential electron transfer from FMN to the HydC [2Fe-2S] cluster and subsequent reduction of a uniquely penta-coordinated HydB [2Fe-2S] cluster require conformational changes, leading to ferredoxin binding and reduction by a [4Fe-4S] cluster in HydB. This work clarifies the electron transfer pathways for a large group of hydrogenases underlying many essential functions in anaerobic microorganisms.
External linksSci Adv / PubMed:35213221 / PubMed Central
MethodsEM (single particle)
Resolution3.0 - 3.2 Å
Structure data

25633

7t2r

EMDB-25633, PDB-7t2r:
Structure of electron bifurcating Ni-Fe hydrogenase complex HydABCSL in FMN-free apo state
Method: EM (single particle) / Resolution: 3.2 Å

25647

7t30

EMDB-25647, PDB-7t30:
Structure of electron bifurcating Ni-Fe hydrogenase complex HydABCSL in FMN/NAD(H) bound state
Method: EM (single particle) / Resolution: 3.0 Å

Chemicals

ChemComp-FES:
FE2/S2 (INORGANIC) CLUSTER

ChemComp-SF4:
IRON/SULFUR CLUSTER

ChemComp-3NI:
NICKEL (III) ION

ChemComp-FCO:
CARBONMONOXIDE-(DICYANO) IRON

ChemComp-NAD:
NICOTINAMIDE-ADENINE-DINUCLEOTIDE / NAD*YM

ChemComp-FMN:
FLAVIN MONONUCLEOTIDE

Source
  • acetomicrobium mobile (bacteria)
KeywordsOXIDOREDUCTASE / hydrogenase complex / electron bifurcation

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