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Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells.

Published version
Peer-reviewed

Type

Article

Change log

Authors

Nam, Dong Heon 
Kornienko, Nikolay 
Heidary, Nina 

Abstract

Hydrogenases (H2 ases) 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 H2 ase through the introduction of a hierarchical inverse opal (IO) TiO2 interlayer. This proton-reducing Si|IO-TiO2 |H2 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-TiO2 |H2 ase to a modified BiVO4 photoanode in a photoelectrochemical (PEC) cell during several hours of irradiation. Connecting the Si|IO-TiO2 |H2 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.

Description

Keywords

hydrogenase, photoelectrochemistry, photosynthesis, silicon, water splitting, Bismuth, Electrochemical Techniques, Electrodes, Hydrogen, Hydrogenase, Light, Photochemical Processes, Photosystem II Protein Complex, Quartz Crystal Microbalance Techniques, Silicon, Solar Energy, Titanium, Vanadates, Water

Journal Title

Angew Chem Int Ed Engl

Conference Name

Journal ISSN

1433-7851
1521-3773

Volume Title

57

Publisher

Wiley
Sponsorship
Christian Doppler Forschungsgesellschaft (unknown)
European Research Council (682833)
Royal Society (NF160054)
EPSRC (1504244)
Biotechnology and Biological Sciences Research Council (1644244)
Engineering and Physical Sciences Research Council (EP/G037221/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)
This work was supported by an ERC Consolidator Grant “MatEnSAP” (D.H.N, J.Z.Z, N.H., E.R.), the University of Cambridge (Vice- Chancellor and Winton scholarships to V.A.), the Royal Society (Newton fellowship to N.K.), the Christian Doppler Research Association and OMV Group (to A.W., E.R.), the EPSRC (Ph.D. studentship to K.P.S, NanoDTC, EP/G037221/1, to K.N., S.H.), the National Research Foundation of Korea (NRF-2015R1A3A2066191 to D.H.N, C.B.P), the German Research foundation (DFG) within the cluster of excellence EXC 314, “UniCat” (to I.Z.). Prof. A. William Rutherford (Imperial College London) is acknowledged for providing a sample of PSII, Prof. Dominic S. Wright for providing the TiCo precatalyst, Marina Ianello and Dr Christine Cavazza for isolating and purifying the hydrogenase and Dr. William E. Robinson for helpful discussions.