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    Light-Driven Water Oxidation Using Polyelectrolyte Layer-by-Layer Chromophore–Catalyst Assemblies
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    † Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States
    ‡ Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
    *E-mail: [email protected]
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2016, 1, 2, 339–343
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    https://doi.org/10.1021/acsenergylett.6b00171
    Published June 21, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    Layer-by-Layer (LbL) polyelectrolyte self-assembly occurs by the alternate exposure of a substrate to solutions of oppositely charged polyelectrolytes or polyions. Here, we report the application of LbL to construct chromophore–catalyst assemblies consisting of a cationic polystyrene-based Ru polychromophore (PS-Ru) and a [Ru(tpy)(2-pyridyl-N-methylbenzimidazole) (OH2)]2+ water oxidation catalyst (RuC), codeposited with poly(acrylic acid) (PAA) as an inert polyanion. These assemblies are deposited onto planar indium tin oxide (ITO, Sn:In2O3) substrates for electrochemical characterization and onto mesoporous substrates consisting of a SnO2/TiO2 core/shell structure atop fluorine doped tin oxide (FTO) for application to light-driven water oxidation in a dye-sensitized photoelectrosynthesis cell. Cyclic voltammetry and ultraviolet–visible absorption spectroscopy reveal that multilayer deposition progressively increases the film thickness on ITO glass substrates. Under an applied bias, photocurrent measurements of the (PAA/PS-Ru)5/(PAA/RuC)5 LbL films formed on FTO//SnO2/TiO2 mesoporous core–shell electrodes demonstrate a clear anodic photocurrent response. Prolonged photoelectrolysis experiments, with the use of a dual working electrode collector–generator cell, reveal production of O2 from the illuminated photoanode with a Faradaic efficiency of 22%. This is the first report to demonstrate the use of polyelectrolyte LbL to construct chromophore–catalyst assemblies for water oxidation.

    Copyright © 2016 American Chemical Society

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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2016, 1, 2, 339–343
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.6b00171
    Published June 21, 2016
    Copyright © 2016 American Chemical Society
    Request reuse permissions

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