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Visible Light-Driven Dye-Sensitized Photocatalytic Hydrogen Production by Porphyrin and its Cyclic Dimer and Trimer: Effect of Multi-Pyridyl-Anchoring Groups on Photocatalytic Activity and Stability

  • Motonori Watanabe*
    Motonori Watanabe
    International Institute for Carbon Neutral Energy Research, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    *E-mail: [email protected]
  • Songmei Sun
    Songmei Sun
    International Institute for Carbon Neutral Energy Research, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    More by Songmei Sun
  • Tatsumi Ishihara
    Tatsumi Ishihara
    International Institute for Carbon Neutral Energy Research, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    Department of Applied Chemistry, Faculty of Engineering, Kyushu University, Nishi-ku, Fukuoka 819-0395, Japan
  • Takuya Kamimura
    Takuya Kamimura
    Institute for Materials Chemistry and Engineering, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
  • Masato Nishimura
    Masato Nishimura
    Institute for Materials Chemistry and Engineering, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
  • , and 
  • Fumito Tani*
    Fumito Tani
    Institute for Materials Chemistry and Engineering, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    *E-mail: [email protected]
    More by Fumito Tani
Cite this: ACS Appl. Energy Mater. 2018, 1, 11, 6072–6081
Publication Date (Web):October 5, 2018
https://doi.org/10.1021/acsaem.8b01113
Copyright © 2018 American Chemical Society

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    Abstract

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    The monomer, dimer, and trimer of 5,15-diphenyl-10,20-di(pyridin-4-yl)porphyrin are used to investigate the multianchoring effect on TiO2 for visible light-driven photocatalytic hydrogen production in a water medium. Further, the porphyrin trimer is prepared and analyzed by nuclear magnetic resonance (NMR) spectroscopy, absorption spectroscopy, electrochemical voltammetry, fast atom bombardment (FAB) mass spectroscopy, and density functional theory (DFT) computation. The results of this study indicate that the peak intensities of the absorption spectra increase as the number of porphyrin units increases, while changes could be barely observed in the highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gaps. The porphyrin dimer in a 1 wt % Pt-loaded TiO2 powder photocatalyst system exhibited optimal hydrogen production performance in a stable state over a period of 80 h and at a superior rate of 1023 μmol·g–1·h–1. Further, the stability of the photocatalytic system was systematically investigated using films containing dyes on 1 wt % Pt-loaded TiO2/FTO. For a film containing the dimer, almost no change was observed in the hydrogen-bond coordination mode of the dimer and the photocurrent during the photocatalytic reaction. However, the photocurrents of the monomer and trimer were altered during visible light irradiation without altering the coordination mode, indicating that the arrangements and orientations of the porphyrins on TiO2 surfaces were altered. These results indicate that the presence of multiple anchoring groups enhance the stability of the photocatalytic system and the rate of hydrogen production.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsaem.8b01113.

    • Absorption spectra of dyes on TiO2 film, difference pulse voltammetry of 13, 0.1 M nBu4NPF6 in 1,1,2,2-tetrachloroethane solution, absorption spectra of soluble species in 1,1,2,2-tetrachloroethane solvent from an aqueous solution after the photocatalytic hydrogen production reaction, the time-course of the turnover numbers per porphyrin unit for hydrogen production, and visible light-driven photocatalytic hydrogen production under dye/Pt–TiO2 film in FTO substrate conditions (PDF)

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