New Paper ‒ Simultaneous Electrosynthesis of Syngas and an Aldehyde
A tandem cell for artificial photosynthesis with CO2 and water as the oxidants and an organic alcohol as the reductant is described. The use of molecular catalysts with high activity and selectivity, in an appropriate cell configuration, leads to electrochemical reduction … Read more
New Paper ‒ A Silane-Derivatized Ru(II) Catalyst for Water Oxidation
The silane-derivatized catalyst, Ru(bda)(L)2 (bda = 2,2′-bipyridine-6,6′-dicarboxylate, L = 4-(6-(triethoxysilyl)hexyl)pyridine), is stabilized on metal oxide electrode surfaces over an extended pH range. It maintains its reactivity on the electrode surface toward electrochemical oxidation over a wide range of conditions. On … Read more
Humboldt Fellowship: Congratulations Jenny Schneider
Congratulations to AMPED EFRC postdoctoral fellow Jenny Schneider, who has been awarded a prestigious Feodor Lynen Research Fellowship from the Humboldt Foundation. The Humboldt Foundation sponsors highly qualified German researchers of all disciplines who wish to conduct research abroad. Jenny Schneider … Read more
Larraín Gandarillas Medal: Congratulations Tom Meyer
Congratulations to former UNC EFRC Director Tom Meyer, who has been awarded the Monsignor Larraín Gandarillas Medal by Pontifica Universidad Católica de Chile. Professor Meyer was presented with the medal during his recent visit to Chile, in recognition of his … Read more
DOE Newsletter Editorial Board: Congratulations Chiung-Wei Huang
Congratulations to Chiung-Wei Huang, 4th year graduate student in the Atkin group and member of the AMPED EFRC Photoanode and Photocathode Teams, who has been accepted to the editorial board of the DOE EFRC quarterly newsletter Frontiers in Energy Research. … Read more
New Paper ‒ A Charge‐Separated State that Lives for Almost a Second
Transparent conductive oxides (TCOs) are widely-used commercially available materials for opto‐electronic applications, yet have received very little attention for dye‐sensitization applications. This paper reports that mesoporous thin films of conductive indium‐doped tin oxide (ITO) nanocrystallites support long‐lived charge separation with … Read more
New Review ‒ Carbon Dioxide Electroreduction
The development of molecular organometallic electrocatalysts for the reduction of carbon dioxide (CO2) is reviewed. Organometallic complexes are a promising subset of the many catalysts capable of electrochemical reduction of carbon dioxide to organic small molecules such as carbon monoxide (CO), formate (HCO2−), and oxalate (C2O42−). The carbon-based supporting ligands of organometallic complexes … Read more
New Paper ‒ Optimization of Photocatalyst Reduction Potentials for Dye-Sensitized HBr Splitting
Dye-sensitized bromide oxidation was investigated using a series of ruthenium polypyridyl photocatalysts anchored to SnO2/TiO2 core/shell mesoporous thin films through 2,2’-bipyridine-4,4’-diphosphonic acid anchoring groups. The ground- and excited-state reduction potentials were tuned over 500 mV by the introduction of electron-withdrawing … Read more
New Paper ‒ Stabilized Photoanodes for Water Oxidation
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
New Paper ‒ Photocatalytic Water Oxidation by a π-Conjugated Chromophore-Catalyst Assembly
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
New Paper ‒ Completing a Charge Transport Chain for Artificial Photosynthesis
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
AMPED EFRC ‒ Congratulations
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
New Paper ‒ Catalytic Interconversion
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
New Paper ‒ Stability of Phosphonate-Derivatized Sensitizers on Metal Oxide Surfaces
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
New Paper ‒ Interfacial Dynamics
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