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Earth-Abundant Molecular Z‑Scheme Photoelectrochemical Cell for Overall Water-Splitting

A push–pull organic dye and a cobaloxime catalyst were successfully cografted on NiO and CuGaO2 to form efficient molecular photocathodes for H2 production with >80% Faradaic efficiency. CuGaO2 is emerging as a more effective p-type semiconductor in photoelectrochemical cells and yields a photoca...

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Published in:Journal of the American Chemical Society 2019-06, Vol.141 (24), p.9593-9602
Main Authors: Windle, Christopher D, Kumagai, Hiromu, Higashi, Masanobu, Brisse, Romain, Bold, Sebastian, Jousselme, Bruno, Chavarot-Kerlidou, Murielle, Maeda, Kazuhiko, Abe, Ryu, Ishitani, Osamu, Artero, Vincent
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Language:English
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Summary:A push–pull organic dye and a cobaloxime catalyst were successfully cografted on NiO and CuGaO2 to form efficient molecular photocathodes for H2 production with >80% Faradaic efficiency. CuGaO2 is emerging as a more effective p-type semiconductor in photoelectrochemical cells and yields a photocathode with 4-fold higher photocurrent densities and 400 mV more positive onset photocurrent potential compared to the one based on NiO. Such an optimized CuGaO2 photocathode was combined with a TaON|CoO x photoanode in a photoelectrochemical cell. Operated in this Z-scheme configuration, the two photoelectrodes produced H2 and O2 from water with 87% and 88% Faradaic efficiency, respectively, at pH 7 under visible light and in the absence of an applied bias, equating to a solar to hydrogen conversion efficiency of 5.4 × 10–3%. This is, to the best of our knowledge, the highest efficiency reported so far for a molecular-based noble metal-free water splitting Z-scheme.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.9b02521