Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 16, Pages 4778-4781Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201410944
Keywords
electropolymerization; photoelectrochemistry; proton-coupled electron transfer; solar fuels; water oxidation
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Funding
- UNC EFRC Center for Solar Fuels, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- Department of Energy Office of Science [DE-AC05-06OR23100]
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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 pH7 phosphate buffer solution. Photogenerated oxygen was measured in real-time by use of a two-electrode cell design.
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