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Updated: Dec 1, 2025

Developing Photosensitizer-Cobaloxime Hybrids for Solar-Driven H2 Production in Aqueous Aerobic Conditions
Published on: October 5, 2019
Photo-recycling the Sacrificial Electron Donor: Towards Sustainable Hydrogen Evolution in a Biphasic System
Peiyu Ge1, Mohamad Hojeij1, Micheál D Scanlon2,3
1Laboratoire d'Électrochimie Physique et Analytique, École Polytechnique Fédérale de Lausanne, EPFL, Valais Wallis, Rue de l'industrie, 17, 1950, SION, Switzerland.
Abstract:
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.
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