title: Photoelectrochemical H2 Evolution with a Hydrogenase Immobilized on a TiO2 -Protected Silicon Electrode.
abstract: The combination of enzymes with semiconductors enables the photoelectrochemical characterization of electron-transfer processes at highly active and well-defined catalytic sites on a light-harvesting electrode surface. Herein, we report the integration of a hydrogenase on a TiO2 -coated p-Si photocathode for the photo-reduction of protons to H2 . The immobilized hydrogenase exhibits activity on Si attributable to a bifunctional TiO2 layer, which protects the Si electrode from oxidation and acts as a biocompatible support layer for the productive adsorption of the enzyme. The p-Si|TiO2 |hydrogenase photocathode displays visible-light driven production of H2 at an energy-storing, positive electrochemical potential and an essentially quantitative faradaic efficiency. We have thus established a widely applicable platform to wire redox enzymes in an active configuration on a p-type semiconductor photocathode through the engineering of the enzyme-materials interface.
authors.affiliation: Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK.|ARC Centre of Excellence for Electromaterials Science, Intelligent Polymer Research Institute/AIIM Faculty, Innovation Campus, University of Wollongong, Wollongong, NSW, 2522, Australia.
authors.forename: Chong-Yong
authors.initials: CY
authors.lastname: Lee
authors.affiliation: Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK.|Fuel Cell Research Center, Korea Institute of Science and Technology (KIST), 02792, Seoul, Republic of Korea.
authors.forename: Hyun S
authors.initials: HS
authors.lastname: Park
authors.affiliation: Metalloproteins Unit, Institut de Biologie Structurale, CEA, CNRS, Université Grenoble Alpes, 38044, Grenoble, France.
authors.forename: Juan C
authors.initials: JC
authors.lastname: Fontecilla-Camps
authors.affiliation: Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK. reisner@ch.cam.ac.uk.
authors.forename: Erwin
authors.initials: E
authors.lastname: Reisner
keywords: TiO2; hydrogen evolution; hydrogenase; photoelectrochemistry; semiconductors