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Light Absorption Properties and Electronic Band Structures of Lead Titanium Oxyfluoride Photocatalysts Pb2Ti4O9F2 and Pb2Ti2O5.4F1.2

  • Haruki Wakayama
    Haruki Wakayama
    Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo 152-8550, Japan
  • Keishu Utimula
    Keishu Utimula
    School of Materials Science, JAIST, Asahidai 1-1, Nomi, Ishikawa 923-1292, Japan
  • Tom Ichibha
    Tom Ichibha
    School of Information Science, JAIST, Asahidai 1-1, Nomi, Ishikawa 923-1292, Japan
    More by Tom Ichibha
  • Ryo Kuriki
    Ryo Kuriki
    Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo 152-8550, Japan
    Japan Society for the Promotion of Science, Kojimachi Business Center Building, 5-3-1 Kojimachi, Chiyoda-ku, Tokyo 102-0083, Japan
    More by Ryo Kuriki
  • Kenta Hongo
    Kenta Hongo
    Research Center for Advanced Computing Infrastructure, JAIST, Asahidai 1-1, Nomi, Ishikawa 923-1292, Japan
    Center for Materials Research by Information Integration, Research and Services Division of Materials Data and Integrated System, National Institute for Materials Science, Tsukuba 305-0047, Japan
    PRESTO, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi-shi, Saitama 322-0012, Japan
    Computational Engineering Applications Unit, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan
    More by Kenta Hongo
  • Ryo Maezono
    Ryo Maezono
    School of Information Science, JAIST, Asahidai 1-1, Nomi, Ishikawa 923-1292, Japan
    Computational Engineering Applications Unit, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan
    More by Ryo Maezono
  • Kengo Oka*
    Kengo Oka
    Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, Bunkyo-ku, Tokyo 112-8551, Japan
    *E-mail: [email protected] (K.O.).
    More by Kengo Oka
  • , and 
  • Kazuhiko Maeda*
    Kazuhiko Maeda
    Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo 152-8550, Japan
    *E-mail: [email protected] (K.M.).
Cite this: J. Phys. Chem. C 2018, 122, 46, 26506–26511
Publication Date (Web):October 29, 2018
https://doi.org/10.1021/acs.jpcc.8b08953
Copyright © 2018 American Chemical Society

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    Abstract

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    Light absorption capability and electronic band structure are both fundamental information for the development of a new photocatalyst. Here, we investigated two oxyfluoride photocatalysts Pb2Ti4O9F2 and Pb2Ti2O5.4F1.2, which were active for H2 evolution in the presence of a sacrificial reagent, by means of X-ray diffraction, UV–visible diffuse reflectance spectroscopy, electrochemical impedance spectroscopy, and density functional theory calculations. Pb2Ti4O9F2 and Pb2Ti2O5.4F1.2 show absorption edges at around 410 and 510 nm, respectively, corresponding to band gaps of 3.0 and 2.4 eV. The different band gap values of the two materials are mainly due to their valence band maximum (VBM); the VBM of Pb2Ti4O9F2 is positioned at approximately 0.9 V more positive than that of Pb2Ti2O5.4F1.2. The significantly different VBM positions in these oxyfluorides could be explained in terms of the orbital interaction between Pb 6s/6p and O 2p in the valence band, where the shorter Pb–O bond in Pb2Ti2O5.4F1.2 reinforced the interaction, leading to more elevated VBM and a narrower band gap.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.8b08953.

    • EDS mapping results, Mott–Schottky plots, and XRD patterns for Pb2Ti4O9F2 and time courses of H2 evolution by Pt-loaded Pb2Ti4O9F2 under UV irradiation (PDF)

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    This article is cited by 32 publications.

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