期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 119, 期 24, 页码 13858-13867出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.5b01442
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]
- 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
Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) use visible light to split water using molecular sensitizers and water oxidation catalysts codeposited onto mesoporous TiO2 electrodes. Despite a high quantum yield of charge injection and low requirement for the catalytic turnover rate, the quantum yield of water splitting in WS-DSPECs is typically low (<1%). Here we examine the charge separation and recombination processes in WS-DSPECs photoanodes functionalized with varying amounts of IrO2 nanoparticle catalyst. Charge extraction and transient open-circuit voltage decay measurements provide insight into the relationship between light intensity, conduction band electron density, open-circuit photovoltage, and recombination time scale. We correlate these results with electrochemical impedance spectroscopy and present the first complete equivalent circuit model for a WS-DSPEC. The data show quantitatively that recombination of photoinjected electrons with oxidized sensitizer molecules and scavenging by the water oxidation catalyst limit the concentration of conduction band electrons and by extension the photo current of WS-DSPECs.
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