Research Topics
| Christophe LegerSummaryAffiliation: Centre National de la Recherche Scientifique Country: France Publications
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Detail Information
Publications
Inhibition and aerobic inactivation kinetics of Desulfovibrio fructosovorans NiFe hydrogenase studied by protein film voltammetryChristophe Leger
Unite de Bioenergetique et Ingenierie des Proteines, Institut de Biologie Structurale et Microbiologie, CNRS UPR9036 et Université de Provence, 31, Chemin Joseph Aiguier, 13402, Marseille, France
J Am Chem Soc 126:12162-72. 2004..This experimental approach could be used to study the reaction of other multicentered metalloenzymes with their gaseous substrates or inhibitors...
Electron flow in multicenter enzymes: theory, applications, and consequences on the natural design of redox chainsChristophe Leger
Laboratoire de Bioenergetique et Ingenierie des Proteines, UPR 9036, CNRS, IBSM and Université de Provence, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 128:180-7. 2006..This suggests an alternative to the idea that redox chains are optimized in terms of speed: evolutionary pressure may have resulted in slowing down intramolecular ET in order to tune the enzyme's "operating potential"...
Direct electrochemistry of redox enzymes as a tool for mechanistic studiesChristophe Leger
Laboratoire de Bioenergetique et Ingenierie des Proteines, CNRS UPR 9036, IBSM, and Universite de Provence, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
Chem Rev 108:2379-438. 2008
Original design of an oxygen-tolerant [NiFe] hydrogenase: major effect of a valine-to-cysteine mutation near the active sitePierre Pol Liebgott
CNRS, Laboratoire de Bioénergétique et Ingénierie des Protéines, Institut de Microbiologie de la Méditerranée, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 133:986-97. 2011..The electrochemical behavior of the V74C mutant toward O(2) is intermediate between that of the WT enzyme from D. fructosovorans and the oxygen-tolerant MBH from Aquifex aeolicus...
Relating diffusion along the substrate tunnel and oxygen sensitivity in hydrogenasePierre Pol Liebgott
Centre National de la Recherche Scientifique, Unité Propre de Recherche 9036, Unite de Bioenergetique et Ingenierie des Proteines, Institut Fédératif de Recherche 88, Institut de Microbiologie de la Mediterranee, Marseille, France
Nat Chem Biol 6:63-70. 2010..We quantitatively define the relations between diffusion, the Michaelis constant for H2 and rates of inhibition, and we demonstrate that certain enzymes are slowly inactivated by O2 because access to the active site is slow...
Dependence of catalytic activity on driving force in solution assays and protein film voltammetry: insights from the comparison of nitrate reductase mutantsVincent Fourmond
Centre National de la Recherche Scientifique, UPR 9036, Unite de Bioenergetique et Ingenierie des Proteines, Institut de Microbiologie de la Mediterranee, and Aix Marseille Universite, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
Biochemistry 49:2424-32. 2010....
Rates of intra- and intermolecular electron transfers in hydrogenase deduced from steady-state activity measurementsSebastien Dementin
Laboratoire de Bioenergetique et Ingenierie des Proteines, CNRS UPR 9036, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 133:10211-21. 2011..This establishes that FeS-to-FeS rate constants are extremely sensitive to the nature and coordination of the centers...
Understanding and tuning the catalytic bias of hydrogenaseAbbas Abou Hamdan
Laboratoire de Bioenergetique et Ingenierie des Proteines, Institut de Microbiologie de la Mediterranee, CNRS and Aix Marseille Université, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 134:8368-71. 2012..We evidence a novel strategy for tuning the catalytic bias of an oxidoreductase, which consists in modulating the rate of a step that is limiting only in one direction of the reaction, without modifying the properties of the active site...
Changing the ligation of the distal [4Fe4S] cluster in NiFe hydrogenase impairs inter- and intramolecular electron transfersSebastien Dementin
Laboratoire de Bioenergetique et Ingenierie des Proteines, CNRS UPR 9036, IBSM and Université de Provence, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 128:5209-18. 2006..This demonstrates that although [4Fe4S] clusters are robust chemical constructs, the direct protein ligands play an essential role in imparting their ability to transfer electrons...
Major Mo(V) EPR signature of Rhodobacter sphaeroides periplasmic nitrate reductase arising from a dead-end species that activates upon reduction. Relation to other molybdoenzymes from the DMSO reductase familyVincent Fourmond
Unite de Bioenergetique et Ingenierie des Proteines, IBSM, UPR 9036, CNRS, 31 Chemin Joseph Aiguier, F 13402 Marseille Cedex 20, France
J Phys Chem B 112:15478-86. 2008..This could be applied to other enzymes for which the question arises as to the catalytic relevance of certain long-lived, spectroscopically characterized species...
Reassessing the strategies for trapping catalytic intermediates during nitrate reductase turnoverVincent Fourmond
Unite de Bioenergetique et Ingenierie des Proteines, Institut de Microbiologie de la Mediterranee, Centre National de la Recherche Scientifique, UPR 9036, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Phys Chem B 114:3341-7. 2010....
Experimental approaches to kinetics of gas diffusion in hydrogenaseFanny Leroux
Centre National de la Recherche Scientifique, Institut de Biologie Structurale et Microbiologie, Unité Propre de Recherche 9036, Unite de Bioenergetique et Ingenierie des Proteines, Marseille, France
Proc Natl Acad Sci U S A 105:11188-93. 2008..Our results demonstrate the necessity of measuring diffusion rates and emphasize the role of side-chain dynamics in determining these...
Introduction of methionines in the gas channel makes [NiFe] hydrogenase aero-tolerantSebastien Dementin
CNRS, Bioenergetique et Ingenierie des Proteines, IMM, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 131:10156-64. 2009..These results show for the first time that it is possible to improve O(2)-tolerance of [NiFe] hydrogenases, making possible the development of biohydrogen production systems...
O(2)-independent formation of the inactive states of NiFe hydrogenaseAbbas Abou Hamdan
Aix Marseille Universite, Centre National de la Recherche Scientifique CNRS, Laboratoire de Bioenergetique et Ingenierie des Proteines, Unité Mixte de Recherche 7281, Institut de Microbiologie de la Mediterranee, Marseille, France
Nat Chem Biol 9:15-7. 2013..Our findings offer new ways toward the understanding of O(2) inactivation and O(2) tolerance in NiFe hydrogenases...
Correcting for electrocatalyst desorption and inactivation in chronoamperometry experimentsVincent Fourmond
Unite de Bioenergetique et Ingenierie des Proteines, IMM, UPR 9036, CNRS, 31 Chemin Joseph Aiguier, F 13402 Marseille Cedex 20, France
Anal Chem 81:2962-8. 2009..This method also applies to experiments where electron transfer is mediated, rather than direct, providing the current is proportional to the time-dependent concentration of catalyst...
Relation between anaerobic inactivation and oxygen tolerance in a large series of NiFe hydrogenase mutantsAbbas Abou Hamdan
Laboratoire de Bioenergetique et Ingenierie des Proteines, Centre National de la Recherche Scientifique, Aix Marseille Universite, Institut de Microbiologie de la Mediterranee, 13402 Marseille Cedex 20, France
Proc Natl Acad Sci U S A 109:19916-21. 2012....
CO disrupts the reduced H-cluster of FeFe hydrogenase. A combined DFT and protein film voltammetry studyCarole Baffert
Bioenergetics and Engineering of Proteins, CNRS, UPR 9036, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 133:2096-9. 2011..Like in the case of oxygen inhibition, the reaction with CO engages the entire H-cluster, rather than only the Fe(2) subsite...
Covalent attachment of FeFe hydrogenases to carbon electrodes for direct electron transferCarole Baffert
CNRS, Aix Marseille Universite, BIP UMR, IMM FR, France
Anal Chem 84:7999-8005. 2012..We also show that covalent attachment has no effect on the catalytic properties of the enzyme, which means that this strategy can also used be for electrochemical studies of the catalytic mechanism...
"Two-step" chronoamperometric method for studying the anaerobic inactivation of an oxygen tolerant NiFe hydrogenaseVincent Fourmond
Laboratoire de Bioenergetique et Ingenierie des Proteines, CNRS, UPR 9036, Institut de Biologie de la Mediterranee and Aix Marseille Universite, 31 Chemin Joseph Aiguier, 13402 Marseille Cedex 20, France
J Am Chem Soc 132:4848-57. 2010..aeolicus . In particular, the activation and inactivation reactions cannot follow the same reaction pathway...
Effects of slow substrate binding and release in redox enzymes: theory and application to periplasmic nitrate reductasePatrick Bertrand
Laboratoire de Bioenergetique et Ingenierie des Proteines, CNRS UPR 9036, IBSM, France
J Phys Chem B 111:10300-11. 2007....
SOAS: a free program to analyze electrochemical data and other one-dimensional signalsVincent Fourmond
Unite de Bioenergetique et Ingenierie des Proteines, UPR 9036, CNRS, 31 Chemin Joseph Aiguier, F 13402 Marseille Cedex 20, France
Bioelectrochemistry 76:141-7. 2009..This free program is available by download from the Internet, and can be installed on computers running any flavor of Unix or Linux, most easily on MacOS X...
Access to the active site of periplasmic nitrate reductase: insights from site-directed mutagenesis and zinc inhibition studiesSebastien Dementin
Laboratoire de Bioenergetique Cellulaire, CEA Cadarache, DSV IBEB SBVME, 13108 St Paul lez Durance Cedex, France
Biochemistry 46:9713-21. 2007..This residue is not conserved in the DMSO reductase superfamily while it is conserved in the periplasmic nitrate reductase family. Zinc inhibition is therefore likely to be specific and restricted to periplasmic nitrate reductases...
Hydrogen-activating enzymes: activity does not correlate with oxygen sensitivityCarole Baffert
, CNRS, , Marseille, France
Angew Chem Int Ed Engl 47:2052-4. 2008
Characterization of two 2[4Fe4S] ferredoxins from Clostridium acetobutylicumOlivier Guerrini
UMR5504, UMR792 Ingénierie des Systèmes Biologiques et des Procédés, CNRS, INRA, INSA, Toulouse F 31400, France
Curr Microbiol 56:261-7. 2008..The physiological function of CAC3527 is discussed...
In Rhodobacter sphaeroides respiratory nitrate reductase, the kinetics of substrate binding favors intramolecular electron transferBettina Frangioni
, CNRS, 31 chemin J. Aiguier, 13402 Marseille, France
J Am Chem Soc 126:1328-9. 2004..Importantly, comparison is made with all Mo enzymes for which PFV data are available, and we emphasize general features of the energetics of the catalytic cycles in enzymes of the DMSO reductase family...
