期刊
NANO LETTERS
卷 13, 期 10, 页码 4802-4809出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl402416s
关键词
Dye-sensitized; stability; atomic layer deposition; photoelectrochemical cell; water splitting; electron transfer
类别
资金
- UNC Energy Frontier Research Center (EFRC) Center for Solar Fuels
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- Research Triangle Solar Fuels Institute
- U.S. Department of Energy [DE-FG26-08NT01925]
Device lifetimes and commercial viability of dye-sensitized solar cells (DSSCs) and dye sensitized photoelectrosynthesis cells (DSPECs) are dependent on the stability of the surface bound molecular chromophore; and catalysts. Maintaining the integrity of the solution-metal oxide interface is especially challenging in DSPECs for water oxidation where it is necessary to perform high numbers of turnovers, under irradiation in an aqueous environment. In this study, we describe the atomic layer deposition (ALD) of TiO2 on nanocrystalline TiO2 prefunctionalized with the dye molecule [Ru(bpy)(2)(4,4'-(PO3H2)bpy)](2+) (RuP) as a strategy to stabilize surface bound molecules. The resulting films are over an order of magnitude more photostable than untreated films and the desorption rate constant exponentially decreases with increased thickness of ALD TiO2 overlayers. However, the injection yield for TiO2-RuP with ALD TiO2 also decreases with increasing overlayer thickness. The combination of decreased injection yield and 95% quenched emission suggests that the ALD TiO2 overlayer acts as a competitive electron acceptor from RuP*, effectively nonproductively quenching the excited state. The ALD TiO2 also increases back electron transfer rates, relative to the untreated film, but is independent of overlayer thickness. The results for TiO2-RuP with an ALD TiO2 overlayer are compared with similar films having ALD Al2O3 overlayers.
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