Effects of Electron Trapping and Protonation on the Efficiency of Water-Splitting Dye-Sensitized Solar Cells

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Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
Cite this: J. Am. Chem. Soc. 2014, 136, 31, 10974–10982
Publication Date (Web):July 14, 2014
Copyright © 2014 American Chemical Society
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Water-splitting dye-sensitized photoelectrochemical (WS-DSPECs) cells employ molecular sensitizers to absorb light and transport holes across the TiO2 surface to colloidal or molecular water oxidation catalysts. As hole diffusion occurs along the surface, electrons are transported through the mesoporous TiO2 film. In this paper we report the effects of electron trapping and protonation in the TiO2 film on the dynamics of electron and hole transport in WS-DSPECs. When the sensitizer bis(2,2′-bipyridine)(4,4′-diphosphonato-2,2′-bipyridine)ruthenium(II) is adsorbed from aqueous acid instead of from ethanol, there is more rapid hole transfer between photo-oxidized sensitizer molecules that are adsorbed from strong acid. However, the photocurrent and open-circuit photovoltage are dramatically lower with sensitizers adsorbed from acid because intercalated protons charge-compensate electron traps in the TiO2 film. Kinetic modeling of the photocurrent shows that electron trapping is responsible for the rapid electrode polarization that is observed in all WS-DSPECs. Electrochemical impedance spectroscopy suggests that proton intercalation also plays an important role in the slow degradation of WS-DSPECs, which generate protons at the anode as water is oxidized to oxygen.

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Sensitizer adsorption isotherms; cyclic voltammetry of electrodes sensitized from DMSO and H2O; current–time data used to obtain Dapp values; fit parameters for curves in Figure 5; photocurrent model fit parameters for DMSO and ethanol in Figure 7; analysis of buffering and diffusion in WS-PECs; emission data from electrodes at negative applied bias (6 pp). This material is available free of charge via the Internet at http://pubs.acs.org.

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