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Lee, Chongx2010,Yong,Park, Hyun S.,Fontecilla‐,Camps, Juan C.,Reisner, Erwin John Wiley and Sons Inc. 2016 Angewandte Chemie Vol.55 No.20
<P><B>Abstract</B></P><P>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 TiO<SUB>2</SUB>‐coated p‐Si photocathode for the photo‐reduction of protons to H<SUB>2</SUB>. The immobilized hydrogenase exhibits activity on Si attributable to a bifunctional TiO<SUB>2</SUB> 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|TiO<SUB>2</SUB>|hydrogenase photocathode displays visible‐light driven production of H<SUB>2</SUB> 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.</P>
Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells
Nam, Dong Heon,Zhang, Jenny Z.,Andrei, Virgil,Kornienko, Nikolay,Heidary, Nina,Wagner, Andreas,Nakanishi, Kenichi,Sokol, Katarzyna P.,Slater, Barnaby,Zebger, Ingo,Hofmann, Stephan,Fontecilla‐,Ca John Wiley and Sons Inc. 2018 Angewandte Chemie Vol.57 No.33
<P><B>Abstract</B></P><P>Hydrogenases (H<SUB>2</SUB>ases) are benchmark electrocatalysts for H<SUB>2</SUB> production, both in biology and (photo)catalysis in vitro. We report the tailoring of a p‐type Si photocathode for optimal loading and wiring of H<SUB>2</SUB>ase through the introduction of a hierarchical inverse opal (IO) TiO<SUB>2</SUB> interlayer. This proton‐reducing Si|IO‐TiO<SUB>2</SUB>|H<SUB>2</SUB>ase photocathode is capable of driving overall water splitting in combination with a photoanode. We demonstrate unassisted (bias‐free) water splitting by wiring Si|IO‐TiO<SUB>2</SUB>|H<SUB>2</SUB>ase to a modified BiVO<SUB>4</SUB> photoanode in a photoelectrochemical (PEC) cell during several hours of irradiation. Connecting the Si|IO‐TiO<SUB>2</SUB>|H<SUB>2</SUB>ase to a photosystem II (PSII) photoanode provides proof of concept for an engineered Z‐scheme that replaces the non‐complementary, natural light absorber photosystem I with a complementary abiotic silicon photocathode.</P>