title: A redox hydrogel protects the O2 -sensitive [FeFe]-hydrogenase from Chlamydomonas reinhardtii from oxidative damage.
abstract: The integration of sensitive catalysts in redox matrices opens up the possibility for their protection from deactivating molecules such as O2 . [FeFe]-hydrogenases are enzymes catalyzing H2 oxidation/production which are irreversibly deactivated by O2 . Therefore, their use under aerobic conditions has never been achieved. Integration of such hydrogenases in viologen-modified hydrogel films allows the enzyme to maintain catalytic current for H2 oxidation in the presence of O2 , demonstrating a protection mechanism independent of reactivation processes. Within the hydrogel, electrons from the hydrogenase-catalyzed H2 oxidation are shuttled to the hydrogel-solution interface for O2 reduction. Hence, the harmful O2 molecules do not reach the hydrogenase. We illustrate the potential applications of this protection concept with a biofuel cell under H2 /O2 mixed feed.
authors.affiliation: Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, 45470 Mülheim an der Ruhr (Germany).
authors.forename: Alaa Alsheikh
authors.initials: AA
authors.lastname: Oughli
authors.affiliation: Analytical Chemistry-Center for Electrochemical Sciences (CES), Ruhr-Universität Bochum, Universitätsstrasse 150, 44780 Bochum (Germany).
authors.forename: Felipe
authors.initials: F
authors.lastname: Conzuelo
authors.affiliation: Lehrstuhl Biochemie der Pflanzen, AG Photobiotechnologie, Ruhr Universität Bochum, Universitätsstrasse 150, 44801 Bochum (Germany).
authors.forename: Martin
authors.initials: M
authors.lastname: Winkler
authors.affiliation: Lehrstuhl Biochemie der Pflanzen, AG Photobiotechnologie, Ruhr Universität Bochum, Universitätsstrasse 150, 44801 Bochum (Germany).
authors.forename: Thomas
authors.initials: T
authors.lastname: Happe
authors.affiliation: Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, 45470 Mülheim an der Ruhr (Germany).
authors.forename: Wolfgang
authors.initials: W
authors.lastname: Lubitz
authors.affiliation: Analytical Chemistry-Center for Electrochemical Sciences (CES), Ruhr-Universität Bochum, Universitätsstrasse 150, 44780 Bochum (Germany).
authors.forename: Wolfgang
authors.initials: W
authors.lastname: Schuhmann
authors.affiliation: Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, 45470 Mülheim an der Ruhr (Germany). olaf.ruediger@cec.mpg.de.
authors.forename: Olaf
authors.initials: O
authors.lastname: Rüdiger
authors.affiliation: Center for Electrochemical Sciences-Molecular Nanostructures, Ruhr-Universität Bochum, Universitätsstrasse 150, 44780 Bochum (Germany). nicolas.plumere@rub.de.
authors.forename: Nicolas
authors.initials: N
authors.lastname: Plumeré
mesh_terms: D016825:Chlamydomonas reinhardtii / Q000201:enzymology*; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate / Q000737:chemistry / Q000378:metabolism*; D006864:Hydrogenase / Q000737:chemistry / Q000378:metabolism*; D007506:Iron-Sulfur Proteins / Q000737:chemistry / Q000378:metabolism*; D008958:Models, Molecular; D015394:Molecular Structure; D010084:Oxidation-Reduction; D010100:Oxygen / Q000737:chemistry / Q000378:metabolism*
chemical_list: D007506:Iron-Sulfur Proteins; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate; C118830:iron hydrogenase; D006864:Hydrogenase; D010100:Oxygen
keywords: O2 protection; biocatalysis; biofuel cells; hydrogenases; viologen hydrogel