Charge Recombination with Fractional Reaction Orders in Water-Splitting Dye-Sensitized Photoelectrochemical Cells

Journal of the American Chemical Society
Pengtao XuThomas E Mallouk

Abstract

In water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs), charge recombination competes with catalytic water oxidation to determine the overall efficiency of the system. The kinetics of these processes have been difficult to understand because transient absorbance (TA) experiments typically show nearly complete charge recombination on the submillisecond time scale; in contrast, electrochemical measurements such as open circuit photovoltage decay suggest a charge recombination time scale that is 2-3 orders of magnitude longer. Here we explore these processes with dye-sensitized nanocrystalline TiO2 and TiO2/Ta2O5 core-shell photoanodes in aqueous electrolytes using TA spectroscopy, intensity-modulated photovoltage spectroscopy (IMVS), and photoelectrochemical impedance spectroscopy (PEIS). The fast recombination rates measured by TA result from strong laser excitation that leads to high electron occupancy in TiO2, whereas IMVS modulates the concentration of charge-separated states near solar irradiance levels. The recombination processes measured by electrochemical methods such as IMVS, PEIS, and transient photovoltage are the discharging of injected electrons in TiO2, as evidenced by the close agreement between ...Continue Reading

References

Oct 30, 2001·Inorganic Chemistry·I Gillaizeau-GauthierG J Meyer
Jan 6, 2009·Journal of the American Chemical Society·W Justin YoungbloodThomas E Mallouk
Sep 14, 2010·Chemical Reviews·Anders HagfeldtHenrik Pettersson
Aug 25, 2016·Nature Chemistry·Ke HuCurtis P Berlinguette
Sep 23, 2016·Journal of the American Chemical Society·M Kyle BrennamanThomas J Meyer
Dec 16, 2016·The Journal of Physical Chemistry Letters·Melissa K GishJohn M Papanikolas
Sep 28, 2017·Physical Chemistry Chemical Physics : PCCP·Hasyiya Karimah AdliShigeru Ikeda
Oct 6, 2017·ACS Applied Materials & Interfaces·Takurou N MurakamiHiroshi Segawa
Feb 6, 2018·Journal of the American Chemical Society·Ludovic Troian-GautierGerald J Meyer

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Citations

Aug 14, 2019·Chemical Communications : Chem Comm·Congcong XueClaudia Turro
Jul 3, 2020·The Journal of Chemical Physics·Naruki HayashiAkira Yamakata
Sep 4, 2019·ChemSusChem·Linfeng PanAnders Hagfeldt
Jun 20, 2020·The Journal of Physical Chemistry. B·Thomas P CheshireFrances A Houle
Aug 21, 2020·Journal of the American Chemical Society·Ke HuGerald J Meyer
Oct 1, 2021·Chemical Society Reviews·Ana Belén Muñoz-GarcíaMarina Freitag

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