Light-Driven Water Splitting with a Molecular Electroassembly-Based Core/Shell Photoanode

An electrochemical procedure for preparing chromophore-catalyst assemblies on oxide electrode surfaces by reductive vinyl coupling is described. On core/shell SnO2/TiO2 nanoparticle oxide films, excitation of the assembly with 1 sun (100 mW cm–2) illumination in 0.1 M H2PO4 –/HPO4 2– at pH 7 with an...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2015-08, Vol.6 (16), p.3213-3217
Main Authors: Sherman, Benjamin D, Ashford, Dennis L, Lapides, Alexander M, Sheridan, Matthew V, Wee, Kyung-Ryang, Meyer, Thomas J
Format: Article
Language:English
Subjects:
catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), hydrogen and fuel cells, electrodes - solar, charge transport, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly)
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Summary:An electrochemical procedure for preparing chromophore-catalyst assemblies on oxide electrode surfaces by reductive vinyl coupling is described. On core/shell SnO2/TiO2 nanoparticle oxide films, excitation of the assembly with 1 sun (100 mW cm–2) illumination in 0.1 M H2PO4 –/HPO4 2– at pH 7 with an applied bias of 0.4 V versus SCE leads to water splitting in a DSPEC with a Pt cathode. Over a 5 min photolysis period, the core/shell photoanode produced O2 with a faradaic efficiency of 22%. Instability of the surface bound chromophore in its oxidized state in the phosphate buffer leads to a gradual decrease in photocurrent and to the relatively modest faradaic efficiencies.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.5b01370