title: Solar water splitting in a molecular photoelectrochemical cell.
abstract: Artificial photosynthesis and the production of solar fuels could be a key element in a future renewable energy economy providing a solution to the energy storage problem in solar energy conversion. We describe a hybrid strategy for solar water splitting based on a dye sensitized photoelectrosynthesis cell. It uses a derivatized, core-shell nanostructured photoanode with the core a high surface area conductive metal oxide film--indium tin oxide or antimony tin oxide--coated with a thin outer shell of TiO2 formed by atomic layer deposition. A "chromophore-catalyst assembly" 1, [(PO3H2)2bpy)2Ru(4-Mebpy-4-bimpy)Rub(tpy)(OH2)](4+), which combines both light absorber and water oxidation catalyst in a single molecule, was attached to the TiO2 shell. Visible photolysis of the resulting core-shell assembly structure with a Pt cathode resulted in water splitting into hydrogen and oxygen with an absorbed photon conversion efficiency of 4.4% at peak photocurrent.
authors.affiliation: Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599.
authors.forename: Leila
authors.initials: L
authors.lastname: Alibabaei
authors.forename: M Kyle
authors.initials: MK
authors.lastname: Brennaman
authors.forename: Michael R
authors.initials: MR
authors.lastname: Norris
authors.forename: Berç
authors.initials: B
authors.lastname: Kalanyan
authors.forename: Wenjing
authors.initials: W
authors.lastname: Song
authors.forename: Mark D
authors.initials: MD
authors.lastname: Losego
authors.forename: Javier J
authors.initials: JJ
authors.lastname: Concepcion
authors.forename: Robert A
authors.initials: RA
authors.lastname: Binstead
authors.forename: Gregory N
authors.initials: GN
authors.lastname: Parsons
authors.forename: Thomas J
authors.initials: TJ
authors.lastname: Meyer
mesh_terms: D002384:Catalysis; D055664:Electrochemical Techniques / Q000379:methods*; D008027:Light; D008956:Models, Chemical; D055668:Photochemical Processes; D012993:Solar Energy; D013997:Time Factors; D014025:Titanium / Q000737:chemistry; D014867:Water / Q000737:chemistry*
chemical_list: D014867:Water; C009495:titanium dioxide; D014025:Titanium