Photoelectrochemical H$_{2}$ Evolution with a Hydrogenase Immobilized on a TiO$_{2}$-Protected Silicon Electrode

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Lee, Chong-Yong 
Park, Hyun S 
Fontecilla-Camps, Juan C 

The integration 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. Here, we report the integration of a hydrogenase on a TiO2-coated p-Si photocathode for the photoreduction 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 biocompatible support layer for the productive adsorption of the enzyme. The p-Si|TiO2|hydrogenase photocathode displays the visible-light driven production of H2 at an energy-storing, positive electrochemical potential and an essentially quantitative faradaic efficiency. We have therefore 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.

TiO2, hydrogen evolution, hydrogenase, photoelectrochemistry, semiconductors
Journal Title
Angewandte Chemie International Edition
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Biotechnology and Biological Sciences Research Council (BB/K010220/1)
This work was supported by the Intra-European Marie-Curie fellowship (to CYL), the BBSRC (BB/K010220/1), the Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy, and the National Foundation for Research, Technology and Development) and the OMV Group (to ER).