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Layered Perovskite Oxyiodide with Narrow Band Gap and Long Lifetime Carriers for Water Splitting Photocatalysis

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    Layered Perovskite Oxyiodide with Narrow Band Gap and Long Lifetime Carriers for Water Splitting Photocatalysis
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    • Kanta Ogawa
      Kanta Ogawa
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), National Institute of Advanced Industrial Science and Technology (AIST), Sakyo-ku, Kyoto 606-8501, Japan
      More by Kanta Ogawa
      Orcidhttps://orcid.org/0000-0002-6995-9848
    • Hajime Suzuki
      Hajime Suzuki
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      More by Hajime Suzuki
      Orcidhttps://orcid.org/0000-0002-8891-2033
    • Chengchao Zhong
      Chengchao Zhong
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      More by Chengchao Zhong
    • Ryota Sakamoto
      Ryota Sakamoto
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      More by Ryota Sakamoto
    • Osamu Tomita
      Osamu Tomita
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      More by Osamu Tomita
    • 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
      Orcidhttps://orcid.org/0000-0001-7429-2200
    • Hiroshi Kageyama*
      Hiroshi Kageyama
      Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan
      *[email protected]
      More by Hiroshi Kageyama
      Orcidhttps://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
      AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), National Institute of Advanced Industrial Science and Technology (AIST), Sakyo-ku, Kyoto 606-8501, Japan
      *[email protected]
      More by Ryu Abe
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 22, 8446–8453
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    https://doi.org/10.1021/jacs.1c02763
    Published May 17, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    The development of semiconductors with narrow band gap and high stability is crucial for achieving solar to chemical energy conversion. Compounds with iodine, which has a high polarizability, have attracted attention because of their narrow band gap and long carrier lifetime, as typified by halide perovskite solar cells; however, they have been regarded as unsuitable for harsh photocatalytic water splitting because iodine is prone to self-oxidation. Here, we demonstrate that Ba2Bi3Nb2O11I, a layered Sillén–Aurivillius oxyiodide, not only has access to a wider range of visible light than its chloride and bromide counterparts, but also functions as a stable photocatalyst, efficiently oxidizing water. Density functional theory calculations reveal that the oxygen 2p orbitals in the perovskite block, rather than the fluorite Bi2O2 block as previously pointed out, anomalously push up the valence band maximum, which can be explained by a modified Madelung potential analysis that takes into account the high polarizability of iodine. In addition, the highly polarizable iodide contributes to longer carrier lifetime of Ba2Bi3Nb2O11I, allowing for a significantly higher quantum efficiency than its chloride and bromide counterparts. Visible-light-driven Z-scheme water splitting was achieved for the first time in an iodine-based system using Ba2Bi3Nb2O11I as an oxygen-evolution photocatalyst. The present study provides a novel approach for incorporating polarizable “soft” anions into building blocks of layered materials to manipulate the band structure and improve the carrier dynamics for visible-light responsive functions.

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    Cite this: J. Am. Chem. Soc. 2021, 143, 22, 8446–8453
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