期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 120, 期 11, 页码 5940-5948出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b00749
关键词
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资金
- Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Energy Biosciences, Department of Energy [DE-FG02-07ER15911, DE-FG02-07ER15909]
- National Science Foundation [DGE1255832]
- Pennsylvania State University Materials Research Institute Nanofabrication Laboratory under National Science Foundation [ECS-0335765]
- Direct For Education and Human Resources
- Division Of Graduate Education [0947962] Funding Source: National Science Foundation
Efficient conversion of solar energy into useful chemical fuels is a major scientific challenge. Water-splitting dye sensitized photoelectrochemical cells (WS-DSPECs) utilize mesoporous oxide supports sensitized with molecular dyes and catalysts to drive the water-splitting reaction. Despite a growing body of work, the overall efficiencies of WS-DSPECs remain low, in large part because of poor electron injection into the conduction band of the oxide support. In this study, we characterize the ultrafast injection dynamics of several proposed oxide supports (TiO2, TiO2/Al2O3, SnO2, SnO2/TiO2) under identical conditions using time-resolved terahertz spectroscopy. In the absence of an Al2O3 overlayer, we observe a two-step injection from the dye singlet state into nonmobile surface traps, which then relax into the oxide conduction band. We also find that, in SnO2-core/TiO2-shell configurations, electron injection into TiO2 trap states occurs rapidly, followed by trapped electrons being released into SnO2 on the hundreds of picoseconds time scale.
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