期刊
ACS APPLIED MATERIALS & INTERFACES
卷 8, 期 26, 页码 16727-16735出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.6b05362
关键词
water-splitting; solar energy; trap states; charge recombination; terahertz spectroscopy
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]
Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) utilize a sensitized metal oxide and a water oxidation catalyst in order to generate hydrogen and oxygen from water. Although the Faradaic efficiency of water splitting is close to unity, the recombination of photogenerated electrons with oxidized dye molecules causes the quantum efficiency of these devices to be low. It is therefore important to understand recombination mechanisms in order to develop strategies to minimize them. In this paper, we discuss the role of proton intercalation in the formation of recombination centers. Proton intercalation forms nonmobile surface trap states that persist on time scales that are orders of magnitude longer than the electron lifetime in TiO2. As a result of electron trapping, recombination with surface-bound oxidized dye molecules occurs. We report a method for effectively removing the surface trap states by mildly heating the electrodes under vacuum, which appears to primarily improve the injection kinetics without affecting bulk trapping dynamics, further stressing the importance of proton control in WS-DSPECs.
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