title: Electro-assembly of a chromophore-catalyst bilayer for water oxidation and photocatalytic water splitting.
abstract: The use of electropolymerization to prepare electrocatalytically and photocatalytically active electrodes for water oxidation is described. Electropolymerization of the catalyst Ru(II)(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.
authors.affiliation: Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States.
authors.forename: Dennis L
authors.initials: DL
authors.lastname: Ashford
authors.forename: Benjamin D
authors.initials: BD
authors.lastname: Sherman
authors.forename: Robert A
authors.initials: RA
authors.lastname: Binstead
authors.forename: Joseph L
authors.initials: JL
authors.lastname: Templeton
authors.forename: Thomas J
authors.initials: TJ
authors.lastname: Meyer
keywords: electropolymerization; photoelectrochemistry; proton-coupled electron transfer; solar fuels; water oxidation