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Elucidation of band alignment in photocatalysts to obtain design strategy based on semiconductor physics

Research Project

Project/Area Number 18H03772
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 21:Electrical and electronic engineering and related fields
Research InstitutionThe University of Tokyo

Principal Investigator

Sugiyama Masakazu  東京大学, 先端科学技術研究センター, 教授 (90323534)

Co-Investigator(Kenkyū-buntansha) 佐藤 正寛  東京大学, 先端科学技術研究センター, 助教 (40805769)
藤井 克司  国立研究開発法人理化学研究所, 光量子工学研究センター, 研究員 (80444016)
Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥44,720,000 (Direct Cost: ¥34,400,000、Indirect Cost: ¥10,320,000)
Fiscal Year 2020: ¥11,180,000 (Direct Cost: ¥8,600,000、Indirect Cost: ¥2,580,000)
Fiscal Year 2019: ¥14,560,000 (Direct Cost: ¥11,200,000、Indirect Cost: ¥3,360,000)
Fiscal Year 2018: ¥18,980,000 (Direct Cost: ¥14,600,000、Indirect Cost: ¥4,380,000)
Keywords光触媒 / 半導体物理 / 界面準位 / バンドアラインメント / 水分解 / 水素 / 光起電力 / 半導体
Outline of Final Research Achievements

Single crystal substrates were used as semiconductor photocatalysts to systematically investigate the effects of defect levels on the semiconductor surface and surface chemical species originating from the electrolyte on the band bending and photovoltage at the semiconductor/electrolyte interface. All of the GaN, SrTiO3, and TiO2 substrates formed a Schottky junction-like band alignment at the interface with an electrolyte, but not only the crystal defects on the semiconductor surface. In addition to the crystal defects on the surface of the semiconductor, surface chemical species also functioned as recombination centers for photoexcited carriers, pinning the Fermi level under light irradiation and preventing the quasi-Fermi level from reaching the potential required for hydrogen and oxygen production. In addition, Pt, which is used as an co-catalyst for hydrogen production, was found to be in ohmic contact with GaN and STO, contrary to expectations based on its work function.

Academic Significance and Societal Importance of the Research Achievements

半導体光触媒の材料探索には,バンド端のエネルギーと水素・酸素発生電位との整合関係が高効率水分解の指標として主に考慮されてきた.本研究により,実際に水素・酸素発生の進行を司る光励起キャリアの擬フェルミエネルギーは,バンド端のエネルギーのみならず半導体/電解液界面での欠陥や半導体表面の化学種を介したキャリアの再結合により,とくに光強度が十分でない場合にピニングされることが明らかになった.本研究で開発した開放電圧を幅広い光強度範囲で観察する手法により,このようなフェルミエネルギーのピニングを定量化することが可能となり,高効率光触媒に必要な半導体の表面処理を最適化する指針が見出された.

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (19 results)

All 2021 2020 2019 2018

All Journal Article (4 results) (of which Peer Reviewed: 4 results) Presentation (15 results) (of which Int'l Joint Research: 7 results,  Invited: 2 results)

  • [Journal Article] Band Bending of nGaN under Ambient H2O Vapor Studied by Xray Photoelectron Spectroscopy2021

    • Author(s)
      Yuki Imazeki, Masahiro Sato, Takahito Takeda, Masaki Kobayashi, Susumu Yamamoto, Iwao Matsuda, Jun Yoshinobu, Masakazu Sugiyama, Yoshiaki Nakano
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: - Issue: 17 Pages: 9011-9019

    • DOI

      10.1021/acs.jpcc.0c11174

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] In-Situ Photoluminescence Analysis of GaN Photoanode During Water Oxidation2021

    • Author(s)
      T. Minegishi, S.; Shizumi, O. Ciftci, T. Endo, Y. Imazeki, Y. Pihosh, M. Sugiyama
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: in press Issue: 19 Pages: 10493-10499

    • DOI

      10.1021/acs.jpcc.1c02005

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Atomistic-Level Description of GaN/Water Interface by a Combined Spectroscopic and First-Principles Computational Approach2020

    • Author(s)
      Sato Masahiro、Imazeki Yuki、Takeda Takahito、Kobayashi Masaki、Yamamoto Susumu、Matsuda Iwao、Yoshinobu Jun、Nakano Yoshiaki、Sugiyama Masakazu
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 23 Pages: 12466-12475

    • DOI

      10.1021/acs.jpcc.0c02192

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] First-principles modeling of GaN(0001)/water interface: Effect of surface charging2019

    • Author(s)
      M. Sato, Y. Imazeki, K. Fujii, Y. Nakano, and M. Sugiyama
    • Journal Title

      The Journal of Chemical Physics

      Volume: 150 Issue: 15 Pages: 154703-154703

    • DOI

      10.1063/1.5086321

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Presentation] GaN薄膜光電極の水分解反応中その場フォトルミネッセンス2020

    • Author(s)
      嶺岸 耕、沈 昊哉、Ciftci Oguz、今関 裕貴、杉山 正和
    • Organizer
      第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Pt担持したSrTiO3(100)面の光電気化学特性2020

    • Author(s)
      沈 昊哉、今関 裕貴、佐藤 正寛、藤井 克司、嶺岸 耕、中野 義昭、杉山 正和
    • Organizer
      第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] GaN電極における光電気化学反応中のフォトルミネッセンス2020

    • Author(s)
      嶺岸耕、沈昊哉、CIFTCI Oguz、今関裕貴、杉山正和
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Pt櫛形電極を形成したSrTiO3モデル光触媒における水分解反応2020

    • Author(s)
      沈 昊哉、遠藤 達朗、嶺岸 耕、杉山 正和
    • Organizer
      第68回応用物理学会春季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Pt櫛型電極を水素生成サイトとするGaNモデル光触媒の解析2020

    • Author(s)
      遠藤 達朗、沈 昊哉、嶺岸 耕、杉山 正和
    • Organizer
      第68回応用物理学会春季学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 光電気化学的水分解におけるSrTiO3の面方位依存性2020

    • Author(s)
      沈昊哉、今関裕貴、スパワンナーンプラパーワット、佐藤正寛、藤 井克司、嶺岸耕、中野義昭、杉山正和
    • Organizer
      応用物理学会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Efficiency enhancement and energy-system application of semiconductor photovoltaic structures: from power generation to solar-fuel productio2019

    • Author(s)
      Masakazu Sugiyama
    • Organizer
      The 2019 Nankai International Symposium on Solar Energy Conversion
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] n-GaN光電極/電解液界面バンドアライメントに及ぼす溶存酸素の影響2019

    • Author(s)
      今関 裕貴、ナーンプラパーワット スパワン、佐藤 正寛、藤井 克司、嶺岸 耕、杉山 正和、中野 義昭
    • Organizer
      応用物理学会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Material-dependent Photoresponse of quasi-Fermi Level in Single-crystalline Photoanodes2019

    • Author(s)
      Supawan Ngamprapawat, Yuki Imazeki, Tsutomu Minegishi, Katsushi Fujii, Masakazu Sugiyama
    • Organizer
      応用物理学会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Efficiency enhancement of semiconductor photovoltaic structures from power generaon to solar-fuel production2019

    • Author(s)
      M. Sugiyama
    • Organizer
      IUMRS-ICA
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Effect of Dissolved O2 on Band Alignment at n-GaN/NaOH Interface2019

    • Author(s)
      Yuki Imazeki,Supawan Ngamprapawat, Masahiro Sato, Katsushi Fujii, Tsutomu Minegishi, Masakazu Sugiyama, Yoshiaki Nakano
    • Organizer
      MRS fall meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Comparison of Light-Intensity-Dependent Open-Circuit Potential among TiO2, SrTiO3 and GaN Single-Crystalline Photoanodes2019

    • Author(s)
      Supawan Ngamprapawat, Yuki Imazeki, Tsutomu Minegishi, Masahiro Sato, Katsushi Fujii, Masakazu Sugiyama
    • Organizer
      MRS fall meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] A Combined Spectroscopic and First-Principles Approach for the Atomistic-Level Description of Semiconductor/Electrolyte Interface2019

    • Author(s)
      Masahiro Sato, Yuki Imazeki, Takahito Takeda, Masaki Kobayashi, Susumu Yamamoto, Iwao Matsuda, Jun Yoshinobu, Yoshiaki Nakano and Masakazu Sugiyama
    • Organizer
      MRS fall meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Impact of surface morphology of Al(Ga)N interlayer for polarization-engineered water splitting photocathode2018

    • Author(s)
      Hiroaki Maruyama, Katsushi Fujii, Yoshiaki Nakano, Masakazu Sugiyama
    • Organizer
      IWN 2018, Nov. 11-16, Kanazawa, Japan, OD13-7
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] The Effect of Illumination on the Geometric Structure of Water Molecules on GaN(0001) Surface2018

    • Author(s)
      Masahiro Sato, Yuki Imazeki, Katsushi Fujii, Yoshiaki Nakano, Masakazu Sugiyama
    • Organizer
      MRS 2018 Fall Meeting, Nov. 25-30, 2018, Boston, USA, CM03.09.
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research

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Published: 2018-04-23   Modified: 2022-01-27  

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