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A push-pull organic dye and a cobaloxime catalyst were successfully cografted on NiO and CuGaO 2 o form efficient molecular photocathodes for H 2 production with &gt;80% Faradaic efficiency. CuGaO 2 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 CuGaO 2 photocathode was combined with a TaON|CoO x photoanode in a photoelectrochemical cell. Operated in this Z-scheme configuration, the two photoelectrodes produced H 2 and O 2 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.

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