Journal article Open Access

Photo-recycling the sacrificial electron donor: Towards sustainable hydrogen evolution in a biphasic system

Ge, Peiyu; Hojeij, Mohamad; Scanlon, Micheál D.; Girault, Hubert H.

H2 may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H2 production requires methodologies to recycle the oxidised donor. Herein, the photo-recycling of decamethylferrocenium cations (DcMFc+) using aqueous core-shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc+ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc+ on the surface of the photo-excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO2 (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc+ due to their lower conduction band energy levels. During photo-recycling, CdS (on CdSe) may be self-oxidised and photo-corrode, instead of water acting as the hole scavenger.

M.D.S. acknowledges the Science Foundation Ireland (SFI) under Grant No. 13/SIRG/2137 and the European Research Council through a Starting Grant (Agreement No. 716792).
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