title: CO disrupts the reduced H-cluster of FeFe hydrogenase. A combined DFT and protein film voltammetry study.
abstract: Carbon monoxide is often described as a competitive inhibitor of FeFe hydrogenases, and it is used for probing H(2) binding to synthetic or in silico models of the active site H-cluster. Yet it does not always behave as a simple inhibitor. Using an original approach which combines accurate electrochemical measurements and theoretical calculations, we elucidate the mechanism by which, under certain conditions, CO binding can cause permanent damage to the H-cluster. Like in the case of oxygen inhibition, the reaction with CO engages the entire H-cluster, rather than only the Fe(2) subsite.
authors.affiliation: Bioenergetics and Engineering of Proteins, CNRS, UPR 9036, 31 chemin Joseph Aiguier, 13402 Marseille Cedex 20, France.
authors.forename: Carole
authors.initials: C
authors.lastname: Baffert
authors.forename: Luca
authors.initials: L
authors.lastname: Bertini
authors.forename: Thomas
authors.initials: T
authors.lastname: Lautier
authors.forename: Claudio
authors.initials: C
authors.lastname: Greco
authors.forename: Kateryna
authors.initials: K
authors.lastname: Sybirna
authors.forename: Pierre
authors.initials: P
authors.lastname: Ezanno
authors.forename: Emilien
authors.initials: E
authors.lastname: Etienne
authors.forename: Philippe
authors.initials: P
authors.lastname: Soucaille
authors.forename: Patrick
authors.initials: P
authors.lastname: Bertrand
authors.forename: Hervé
authors.initials: H
authors.lastname: Bottin
authors.forename: Isabelle
authors.initials: I
authors.lastname: Meynial-Salles
authors.forename: Luca
authors.initials: L
authors.lastname: De Gioia
authors.forename: Christophe
authors.initials: C
authors.lastname: Léger
mesh_terms: D002248:Carbon Monoxide / Q000737:chemistry*; D020134:Catalytic Domain; D004563:Electrochemistry; D006864:Hydrogenase / Q000737:chemistry*; D010084:Oxidation-Reduction; D011789:Quantum Theory
chemical_list: D002248:Carbon Monoxide; D006864:Hydrogenase