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• W2582873633 abstract "Improving stability and slowing charge recombination are some of the greatest challenges in the development of dye-sensitized photoelectrochemical cells (DSPECs) for solar fuels production. We have investigated the effect of encasing dye molecules in varying thicknesses of Al2O3 deposited by atomic layer deposition (ALD) before catalyst loading on both the stability and the charge transfer dynamics in organic dye-sensitized TiO2 photoanodes containing iridium-based molecular water-oxidation catalysts. In the TiO2|dye|Al2O3|catalyst electrodes, a sufficiently thick ALD layer protects the perylene-3,4-dicarboximide (PMI) chromophores from degradation over several weeks of exposure to light. The insulating capacity of the layer allows a higher photocurrent in the presence of ALD while initial charge injection is slowed by only 1.6 times, as observed by femtosecond transient absorption spectroscopy. Rapid picosecond-scale catalyst oxidation is observed in the presence of a dinuclear catalyst, IrIr, but is slowed to tens of picoseconds for a mononuclear catalyst, IrSil, that incorporates a long linker. Photoelectrochemical experiments demonstrate higher photocurrents with IrSil compared to IrIr, which show that recombination is slower for IrSil, while higher photocurrents with IrIr upon addition of ALD layers confirm that ALD successfully slows charge recombination. These findings demonstrate that, beyond stability improvements, ALD can contribute to tuning charge transfer dynamics in photoanodes for solar fuels production and may be particularly useful for slowing charge recombination and accounting for varying charge transfer rates based on the molecular structures of incorporated catalysts." @default.
• W2582873633 created "2017-02-03" @default.
• W2582873633 creator A5017540203 @default.
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• W2582873633 creator A5064040856 @default.
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• W2582873633 creator A5072522213 @default.
• W2582873633 creator A5074510664 @default.
• W2582873633 creator A5087804603 @default.
• W2582873633 date "2017-02-10" @default.
• W2582873633 modified "2023-09-25" @default.
• W2582873633 title "Photodriven Oxidation of Surface-Bound Iridium-Based Molecular Water-Oxidation Catalysts on Perylene-3,4-dicarboximide-Sensitized TiO₂ Electrodes Protected by an Al₂O₃ Layer" @default.
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