Electro‐assembly of a Chromophore–Catalyst Bilayer for Water Oxidation and Photocatalytic Water Splitting |
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Authors: | Dr. Dennis L. Ashford Dr. Benjamin D. Sherman Dr. Robert A. Binstead Prof. Joseph L. Templeton Prof. Thomas J. Meyer |
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Affiliation: | Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States |
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Abstract: | The use of electropolymerization to prepare electrocatalytically and photocatalytically active electrodes for water oxidation is described. Electropolymerization of the catalyst RuII(bda)(4‐vinylpyridine)2 (bda=2,2′‐bipyridine‐6,6′‐dicarboxylate) on planar electrodes results in films containing semirigid polymer networks. In these films there is a change in the water oxidation mechanism compared to the solution analogue from bimolecular to single‐site. Electro‐assembly construction of a chromophore–catalyst structure on mesoporous, nanoparticle TiO2 films provides the basis for a dye‐sensitized photoelectrosynthesis cell (DSPEC) for sustained water splitting in a pH 7 phosphate buffer solution. Photogenerated oxygen was measured in real‐time by use of a two‐electrode cell design. |
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Keywords: | electropolymerization photoelectrochemistry proton‐coupled electron transfer solar fuels water oxidation |
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