Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells.
Nam, Dong Heon
Fontecilla-Camps, Juan C
Park, Chan Beum
Angewandte Chemie (International ed. in English)
John Wiley & Sons Ltd.
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Nam, D. H., Zhang, J., Andrei, V., Kornienko, N., Heidary, N., Wagner, A., Nakanishi, K., et al. (2018). Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells.. Angewandte Chemie (International ed. in English), 57 (33), 10595-10599. https://doi.org/10.1002/anie.201805027
Hydrogenases (H2ases) are benchmark electrocatalysts in 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 by 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 complementary 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 Zscheme that replaces the non-complementary, natural light absorber photosystem I with a complementary abiotic silicon photocathode.
Vanadates, Hydrogen, Bismuth, Titanium, Silicon, Water, Photosystem II Protein Complex, Hydrogenase, Electrodes, Solar Energy, Light, Electrochemical Techniques, Photochemical Processes, Quartz Crystal Microbalance Techniques
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.
Christian Doppler Forschungsgesellschaft (unknown)
ECH2020 EUROPEAN RESEARCH COUNCIL (ERC) (682833)
Royal Society (NF160054)
External DOI: https://doi.org/10.1002/anie.201805027
This record's URL: https://www.repository.cam.ac.uk/handle/1810/283408
Attribution 4.0 International
Licence URL: https://creativecommons.org/licenses/by/4.0/