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    Article

    Conduction Band Control of Oxyhalides with a Triple-Fluorite Layer for Visible Light Photocatalysis
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    • Akinobu Nakada
      Akinobu Nakada
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      PRESTO, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012, Japan
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      Orcidhttp://orcid.org/0000-0001-6670-5044
    • Daichi Kato
      Daichi Kato
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      More by Daichi Kato
      Orcidhttp://orcid.org/0000-0002-1600-4095
    • Ryky Nelson
      Ryky Nelson
      Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52056 Aachen, Germany
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    • Hikaru Takahira
      Hikaru Takahira
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Masayoshi Yabuuchi
      Masayoshi Yabuuchi
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Masanobu Higashi
      Masanobu Higashi
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Hajime Suzuki
      Hajime Suzuki
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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      Orcidhttp://orcid.org/0000-0002-8891-2033
    • Maria Kirsanova
      Maria Kirsanova
      Advanced Imaging Core Facility, Skolkovo Institute of Science and Technology, Nobel str. 3, 121205 Moscow, Russia
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    • Naoji Kakudou
      Naoji Kakudou
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Cédric Tassel
      Cédric Tassel
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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    • Takafumi Yamamoto
      Takafumi Yamamoto
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
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      Orcidhttp://orcid.org/0000-0002-7960-1014
    • Craig M. Brown
      Craig M. Brown
      Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States
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    • Richard Dronskowski
      Richard Dronskowski
      Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52056 Aachen, Germany
      Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, 7098 Liuxian Blvd, Nanshan District, Shenzhen, China
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      Orcidhttp://orcid.org/0000-0002-1925-9624
    • Akinori Saeki
      Akinori Saeki
      Department of Applied Chemistry, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
      More by Akinori Saeki
      Orcidhttp://orcid.org/0000-0001-7429-2200
    • Artem Abakumov
      Artem Abakumov
      Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Nobel str. 3, 121205 Moscow, Russia
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      Orcidhttp://orcid.org/0000-0002-7135-4629
    • Hiroshi Kageyama*
      Hiroshi Kageyama
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      CREST, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012, Japan
      *Email [email protected] (H.K.).
      More by Hiroshi Kageyama
      Orcidhttp://orcid.org/0000-0002-3911-9864
    • Ryu Abe*
      Ryu Abe
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      CREST, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012, Japan
      *Email [email protected] (R.A.).
      More by Ryu Abe
      Orcidhttp://orcid.org/0000-0001-8592-076X
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 6, 2491–2499
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    https://doi.org/10.1021/jacs.0c10288
    Published January 8, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    The discovery of building blocks offers new opportunities to develop and control properties of extended solids. Compounds with fluorite-type Bi2O2 blocks host various properties including lead-free ferroelectrics and photocatalysts. In this study, we show that triple-layered Bi2MO4 blocks (M = Bi, La, Y) in Bi2MO4Cl allow, unlike double-layered Bi2O2 blocks, to extensively control the conduction band. Depending on M, the Bi2MO4 block is truncated by Bi–O bond breaking, resulting in a series of n-zigzag chain structures (n = 1, 2, ∞ for M = Bi, La, Y, respectively). Thus, formed chain structures are responsible for the variation in the conduction band minimum (−0.36 to −0.94 V vs SHE), which is correlated to the presence or absence of mirror symmetry at Bi. Bi2YO4Cl shows higher photoconductivity than the most efficient Bi2O2-based photocatalyst with promising visible-light photocatalytic activity for water splitting. This study expands the possibilities of thickening (2D to 3D) and cutting (2D to 1D) fluorite-based blocks toward desired photocatalysis and other functions.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.0c10288.

    • XRD patterns, SAED patterns, UV–vis DRS, PYS, calculated DOS, SEM images, structural analysis from Rietveld refinement, and photocatalytic activities of Bi2MO4Cl (PDF)

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    CCDC 2017968 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cite this: J. Am. Chem. Soc. 2021, 143, 6, 2491–2499
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