Stabilized photoanodes for light-driven water oxidation were prepared on nanoparticle core/shell electrodes with surface-stabilized donor–acceptor chromophores, a water oxidation catalyst, and an electron-transfer mediator. For the electrode, fluorine-doped tin oxide FTO|SnO2/TiO2|-Org1-|1.1 nm Al2O3|-RuP2+-WOC (water oxidation catalyst) with Org1 (1-cyano-2-(4-(diphenylamino)phenyl)vinyl)phosphonic acid), … Read more
The organic chromophore, 2,2′-(benzo[c][1,2,5]thiadiazole-4,7-diyl)bis(thiophene-3-carboxylic acid), was prepared and investigated along with metal complex [Ru(bda)(pyP)2] (bda = 2,2’-bipyridine-6,6’-dicarboxylate; pyP = 3-(pyridine-4-yloxy)propyl)phosphonic acid), for light-driven water splitting in dye-sensitized photoelectrochemical cells. The resulting co-loaded organic chromophore plus catalyst surface assembly was evaluated … Read more
A ruthenium polypyridyl chromophore with electronically isolated triarylamine substituents models the role of tyrosine in the electron transport chain in photosystem II. When bound to the surface of a TiO2 electrode, electron injection from a Ru(II) Metal-to-Ligand Charge Transfer (MLCT) excited … Read more
The Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED) has been awarded an additional two years of support from the U.S. Department of Energy Office of Science, Office of Basic Energy Sciences. The focus for 2018-2020 will be on … Read more
Surface catalytic interconversion of hydroquinone and 1,4-benzoquinone occur at a fluorine-doped tin oxide electrode (FTO) modified by the addition of the surface-bound couple, [Os(bpy)2((4,4’-PO3H2)2bpy)]3+/2+. Significant rate enhancements are observed with added solution buffers – phosphate, acetate, and citrate – and … Read more
A series of Ru(II) polypyridyl complexes were evaluated under electrochemically oxidative conditions, which generates the Ru(III) oxidation state and mimics the harsh conditions in dye-sensitized solar cells, to develop fundamental insights into the factors governing molecular sensitizer surface stability. Results … Read more
Interfacial dynamics following photoexcitation of a water oxidation assembly on nanocrystalline TiO2 electrodes have been investigated. Transient absorption measurements reveal that electron injection occurs with high efficiency but that hole transfer to the catalyst, which occurs on the electrochemical time … Read more