Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells

作者：Dong Heon Nam, Jenny Zhang, Virgil Andrei, Nikolay Kornienko, Nina Heidary, Andreas Wagner, Kenichi Nakanishi, Katarzyna P. Sokol, Barnaby Slater, Ingo Zebger, Stephan Hofmann, Juan Carlos Fontecilla-Camps, Chan Beum Park, Erwin Reisner · 发表于：Angewandte Chemie International Edition · 年份：2018 · DOI：10.1002/anie.201805027 · 被引用次数：113 · 研究领域：Electrocatalysts for Energy Conversion、Metalloenzymes and iron-sulfur proteins、Photosynthetic Processes and Mechanisms

Abstract Hydrogenases (H2ases) are benchmark electrocatalysts for H2 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 H2ase through the introduction of a hierarchical inverse opal (IO) TiO2 interlayer. This proton‐reducing Si|IO‐TiO2|H2ase photocathode is capable of driving overall water splitting in combination with a photoanode. We demonstrate unassisted (bias‐free) water splitting by wiring Si|IO‐TiO2|H2ase to a modified BiVO4 photoanode in a photoelectrochemical (PEC) cell during several hours of irradiation. Connecting the Si|IO‐TiO2|H2ase 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.