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[摘要]：Orthorhombic Nb2O5 nanocrystalline films functionalized with [Ru(bpy)(2)(4,4'-(PO3H2)(2)bpy)](2+) were used as the photo-anode in dye-sensitized photoelectrosynthesis cells (DSPEC) for hydrogen generation. A set of experiments to establish key properties conduction band, trap state distribution, interfacial electron transfer dynamics, and DSPEC efficiency were undertaken to develop a general protocol for future semiconductor evaluation and for comparison with other wide-band-gap semiconductors. We have found that, for a T-phase orthorhombic Nb2O5 nanocrystalline film, the conduction band potential is slightly positive (<0.1 eV), relative to that for anatase TiO2. Anatase TiO2 has a wide distribution of trap states including deep trap and band-tail trap states. Orthorhombic Nb2O5 is dominated by shallow band-tail trap states. Trap state distributions, conduction band energies, and interfacial barriers appear to contribute to a slower back electron transfer rate, lower injection yield on the nanosecond time scale, and a lower open-circuit voltage (V-oc) for orthorhombic Nb2O5, compared to anatase TiO2. In an operating DSPEC, with the ethylenediaminetetraacetic tetra-anion (EDTA(4-)) added as a reductive scavenger, H-2 quantum yield and photostability measurements show that Nb2O5 is comparable, but not superior, to TiO2. |
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