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Development of artificial photosynthesis system driven by interfacial photo-excitation process

Research Project

Project/Area Number 18H02055
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionTokyo Institute of Technology

Principal Investigator

宮内 雅浩  東京工業大学, 物質理工学院, 教授 (60443230)

Project Period (FY) 2018-04-01 – 2023-03-31
Project Status Granted (Fiscal Year 2022)
Budget Amount *help
¥16,900,000 (Direct Cost: ¥13,000,000、Indirect Cost: ¥3,900,000)
Fiscal Year 2022: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Fiscal Year 2021: ¥5,070,000 (Direct Cost: ¥3,900,000、Indirect Cost: ¥1,170,000)
Fiscal Year 2020: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2019: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Fiscal Year 2018: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Keywords光触媒 / 半導体 / 可視光 / 界面電荷移動 / 人工光合成 / 界面 / 励起
Outline of Annual Research Achievements

ナノクラスター/半導体複合体における界面電荷移動遷移(Interfacial Charge Transfer: IFCT)を用い、可視光応答光触媒を開発する。IFCTとして、半導体価電子帯からクラスターへの遷移(Band to Oxidant Charge Transfer: BOCT)と、クラスターから半導体の伝導帯への遷移(Reductant to Band Charge Transfer: RBCT)が知られる。本研究では、SrTiO3基板上にパルスレーザー堆積法とフォトリソグラフィー法によって成膜したCr2O3のパターン膜において、RBCT遷移が起こることをケルビンプローブ顕微鏡で明らかにし、さらにRBCT遷移で励起した電子と正孔の反応サイトについて、光触媒反応による粒子析出を原子間力顕微鏡で追跡することで明らかにした。具体的には、Cr2O3/SrTiO3のパターン化膜を水溶液に浸漬し励起光照射下のもと、酸化反応はマンガンイオンから酸化マンガンの析出、還元反応は金イオンから金を析出させ、酸化マンガンや金の析出する場所によって酸化サイトと還元サイトを特定した。この結果、活性サイトはいずれもパターン膜の界面(エッジ)の部分で、酸化マンガンはCr2O3側へ、金はSrTiO3に析出したことから、前者が酸化サイト、後者が還元サイトであった。すなわち、Cr2O3からSrTiO3にRBCT遷移することによって、前者に正孔が、後者に電子が生成することが示唆された。また、粒子析出の範囲がパターン膜エッジから数十ナノメートルであることから、電子と正孔の拡散距離も明らかにすることができた。プローブ顕微鏡技術と良く定義されたパターン化膜をもとに、異種半導体間での電荷移動を可視化することに成功した。

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

良く定義されたパターン化膜をもとに、Cr2O3とSrTiO3間の電荷移動をケルビンプローブ顕微鏡、原子間力顕微鏡で明らかにすることができ、論文に成果を発表することができた(J. Mater. Chem. A誌)。また、電子、正孔の拡散距離を把握することにも成功し、今後の人工光合成反応実現に向けたナノ粒子開発の基本設計指針を確立することができた。すなわち、SrTiO3やTiO2の半導体に、Cr2O3やCuOを数十ナノメートル以下のサイズのクラスター状で担持することが有効である指針が得られた。この指針は次年度研究につながる大きな成果と考える。

Strategy for Future Research Activity

これまでに得られた知見をもとに、次年度は人口光合成反応、すわなち、水分解に応用する。IFCTプロセスによる水分解を達成するため、水素生成(カソード反応)はBOCT遷移、酸素生成(アノード反応)はRBCT遷移を用いる。いずれもTiO2やSrTiO3半導体微粒子をベースに、IFCTを誘起すべくナノクラスターを担持する。具体的にはBOCT遷移ではCuOナノクラスター、RBCT遷移ではCr2O3ナノクラスターをTiO2やSrTiO3の半導体粒子の表面に担持し、電極化する。電極化においては、半導体粒子の透明導電性基盤へのスクリーン印刷、焼成、含浸法によるナノクラスター担持の順に作製する。得られた電極について、X線回折による結晶構造の解析、走査型および透過型電子顕微鏡による微細組織の観察、X線光電子分光による化学状態、蛍光X線分光による化学組成の分析をおこなう。得られた電極のうち、CuOナノクラスターを半導体に担持した電極をカソード極とし、可視光を照射した際の電流値と水素生成量を分析する。一方、Cr2O3ナノクラスターを半導体に担持した電極をアノード極とし、可視光を照射した場合の電流値と酸素生成量を分析する。水素生成、酸素生成能を高めるため、半導体粒子の粒径や結晶性、ナノクラスターの担持量、電極にした際の膜厚などを最適化する。また、単色光を用いて光電流のアクションスペクトルを分析し、水分解反応の照射光波長依存性を調べることで反応に有効な波長領域を検証する。また、光触媒反応によって生成した分子の起源を明らかにするため、同位体とガスクロマトグラフ質量分析計を用いた解析をおこなう。

Report

(4 results)
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • 2018 Annual Research Report

Research Products

(33 results)

All 2022 2021 2020 2019 2018 Other

All Int'l Joint Research (1 results) Journal Article (16 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 16 results,  Open Access: 5 results) Presentation (15 results) (of which Int'l Joint Research: 10 results,  Invited: 10 results) Book (1 results)

  • [Int'l Joint Research] Central South University(中国)

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Direct imaging of visible-light-induced one-step charge separation at the chromium oxide/strontium titanate interface2022

    • Author(s)
      Wardhana Aufandra Cakra、Yasuhara Sou、Yu Min-Wen、Yamaguchi Akira、Nagao Tadaaki、Ishii Satoshi、Miyauchi Masahiro
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 10 Pages: 752-761

    • DOI

      10.1039/d1ta08950a

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Visible-Light-Induced CO2 Reduction by Mixed-Valence Tin Oxide2021

    • Author(s)
      Liu Yang-Shin、Yamaguchi Akira、Yang Yue、Abe Hideki、Ueda Shigenori、Tanabe Toyokazu、Miyauchi Masahiro
    • Journal Title

      ACS Applied Energy Materials

      Volume: 4 Pages: 13415-13419

    • DOI

      10.1021/acsaem.1c02896

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Active site separation of photocatalytic steam reforming of methane using a gas-phase photoelectrochemical system2021

    • Author(s)
      Kujirai Tomoki、Yamaguchi Akira、Fujita Takeshi、Abe Hideki、Miyauchi Masahiro
    • Journal Title

      Chemical Communications

      Volume: 57 Pages: 8007-8010

    • DOI

      10.1039/d1cc02914b

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Fabrication of Hydrogen Boride Thin Film by Ion Exchange in MgB22021

    • Author(s)
      T. Hirabayashi, S. Yasuhara, S. Shoji, A. Yamaguchi, H. Abe, S. Ueda, H. Zhu, T. Kondo, and M. Miyauchi
    • Journal Title

      Molecules

      Volume: 26 Pages: 6212-6212

    • DOI

      10.3390/molecules26206212

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Temperature dependence on bandgap of semiconductor photocatalysts2020

    • Author(s)
      Y. Cho, A. Yamaguchi, R. Uehara, S. Yasuhara, T. Hoshina, M. Miyauchi
    • Journal Title

      The Journal of Chemical Physics

      Volume: 152 Pages: 231101-231101

    • DOI

      10.1063/5.0012330

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Acid Assisted Synthesis of HB Sheets through Exfoliation of MgB2 Bulk in Organic Media2020

    • Author(s)
      Kawamura Reiya、Yamaguchi Akira、Shimada Chika、Ishibiki Ryota、Fujita Takeshi、Kondo Takahiro、Miyauchi Masahiro
    • Journal Title

      Chemistry Letters

      Volume: 49 Pages: 1194-1196

    • DOI

      10.1246/cl.200203

    • NAID

      130007923163

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Green light active photocatalyst for complete oxidation of organic molecules2020

    • Author(s)
      Yang Yue、Yamaguchi Akira、Jiang Haoyang、van der Kooy Annabel、Okunaka Sayuri、Hosogai Mariko、Tokudome Hiromasa、Miyauchi Masahiro
    • Journal Title

      Chemical Communications

      Volume: 56 Pages: 9210-9213

    • DOI

      10.1039/d0cc03279d

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Antiviral Effect of Visible Light-Sensitive CuxO/TiO2 Photocatalyst2020

    • Author(s)
      Miyauchi Masahiro、Sunada Kayano、Hashimoto Kazuhito
    • Journal Title

      Catalysts

      Volume: 10 Pages: 1093-1093

    • DOI

      10.3390/catal10091093

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Visible-light-driven dry reforming of methane using a semiconductor-supported catalyst2020

    • Author(s)
      Cho Yohei, Shoji Shusaku, Yamaguchi Akira, Hoshina Takuya, Fujita Takeshi, Abe Hideki, Miyauchi Masahiro
    • Journal Title

      Chemical Communications

      Volume: 56 Pages: 4611-4614

    • DOI

      10.1039/d0cc00729c

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Visible-light-driven photocatalysis via reductant-to-band charge transfer in Cr(III) nanocluster-loaded SrTiO3 system2020

    • Author(s)
      Cakra Wardhana Aufandra、Yamaguchi Akira、Shoji Shusaku、Liu Min、Fujita Takeshi、Hitosugi Taro、Miyauchi Masahiro
    • Journal Title

      Applied Catalysis B: Environmental

      Volume: 270 Pages: 118883-118883

    • DOI

      10.1016/j.apcatb.2020.118883

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Photoinduced hydrogen release from hydrogen boride sheets2019

    • Author(s)
      Reiya Kawamura, Nguyen Thanh Cuong, Takeshi Fujita, Ryota Ishibiki, Toru Hirabayashi, Akira Yamaguchi, Iwao Matsuda, Susumu Okada, Takahiro Kondo, Masahiro Miyauchi
    • Journal Title

      Nature Communications

      Volume: 10 Pages: 4880-4880

    • DOI

      10.1038/s41467-019-12903-1

    • NAID

      120007127794

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Synergistic photothermal and photochemical partial oxidation of methane over noble metals incorporated in mesoporous silica2019

    • Author(s)
      Jiang Haoyang、Peng Xiaobo、Yamaguchi Akira、Fujita Takeshi、Abe Hideki、Miyauchi Masahiro
    • Journal Title

      Chemical Communications

      Volume: 55 Pages: 13765-13768

    • DOI

      10.1039/c9cc06170c

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Optical properties of single crystalline copper iodide with native defects: Experimental and density functional theoretical investigation2019

    • Author(s)
      Koyasu Satoshi、Umezawa Naoto、Yamaguchi Akira、Miyauchi Masahiro
    • Journal Title

      Journal of Applied Physics

      Volume: 125 Pages: 115101-115101

    • DOI

      10.1063/1.5082865

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Growth of Large Single Crystals of Copper Iodide by a Temperature Difference Method Using Feed Crystal Under Ambient Pressure2018

    • Author(s)
      Koyasu Satoshi、Umezawa Naoto、Baniecki John D.、Yamaguchi Akira、Miyauchi Masahiro
    • Journal Title

      Crystal Growth & Design

      Volume: 18 Pages: 6748-6756

    • DOI

      10.1021/acs.cgd.8b01024

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Visible-Light-Active Photoelectrochemical Z-Scheme System Based on Top 5 Clarke-Number Elements2018

    • Author(s)
      Miyamoto Hironao、Matsuzaki Kosuke、Yamaguchi Akira、Miyauchi Masahiro
    • Journal Title

      ACS Applied Energy Materials

      Volume: 1 Pages: 5954-5959

    • DOI

      10.1021/acsaem.8b00978

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photocatalytic CO2 Reduction Using a Pristine Cu2ZnSnS4 Film Electrode under Visible Light Irradiation2018

    • Author(s)
      Yoshida Toshiki、Yamaguchi Akira、Umezawa Naoto、Miyauchi Masahiro
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 Pages: 21695-21702

    • DOI

      10.1021/acs.jpcc.8b04241

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Presentation] Elucidation of Interfacial Charge Excitation in Visible-light-active Cr2O3/SrTiO3 Photocatalyst System2021

    • Author(s)
      Aufandra Cakra Wardhana, Satoshi Ishii, Sou Yasuhara, Akira Yamaguchi, Masahiro Miyauchi
    • Organizer
      電気化学会第88回大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Antimicrobial Effect of Photocatalyst and Application to Products2021

    • Author(s)
      M Miyauchi
    • Organizer
      8th International Conference for Universal Design in the Cloud 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] TiO2-based Photocatalyst for Gas-Phase CO2 Recycling2021

    • Author(s)
      Masaru Kushida, Akira Yamaguchi, Masahiro Miyauchi
    • Organizer
      Materials Research Meeting 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Reaction site Separation of Photocatalytic Steam Reforming of Methane With Gas-Phase Photoelectrochemical System2021

    • Author(s)
      Tomoki Kujirai, Akira Yamaguchi, Takeshi Fujita, Hideki Abe, Masahiro Miyauchi
    • Organizer
      Materials Research Meeting 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Current situation on photocatalytic technology in Japan2020

    • Author(s)
      M. Miyauchi
    • Organizer
      Committee of Asian Standardization for Photocatalytic Material and Products (CASP2020)
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Bandgap widening of BiVO4 by diluting Bi orbital component for higher oxidation activity2020

    • Author(s)
      Yue Yang, Akira Yamaguchi, Yohei Cho, Sayuri Okunaka, Hiromasa Tokudome, Masahiro Miyauchi
    • Organizer
      第25回シンポジウム「光触媒反応の最近の展開」
    • Related Report
      2020 Annual Research Report
  • [Presentation] Visible-Light-Active Photocatalysis over Chromium (III)-grafted Strontium Titanate2019

    • Author(s)
      Aufandra Cakra Wardhana, Akira Yamaguchi, Shusaku Shoji, Taro Hitosugi, Masahiro Miyauchi
    • Organizer
      2019年電気化学秋季大会, Sep. 2019.
    • Related Report
      2019 Annual Research Report
  • [Presentation] Metal-oxide-bases photocatalyst for energy and environment,2019

    • Author(s)
      M. Miyauchi
    • Organizer
      Tokyo Institute of Technology and Imperial College London's 2nd Workshop on Plastic Electronics
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photo-induced Dry Reforming of Methane Using Metal Nanoparticles/ Metal Oxide Photocatalysts2019

    • Author(s)
      Masahiro Miyauchi, Shusaku Shoji, Yohei Cho, Akira Yamaguchi, Takeshi Fujita, Hideki Abe
    • Organizer
      Collaborative Conference on Advanced Materials 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photocatalytic Uphill Conversion of Natural Gas Reforming2019

    • Author(s)
      Masahiro Miyauchi, Shusaku Shoji, Yohei Cho, Akira Yamaguchi, Takeshi Fujita, Hideki Abe
    • Organizer
      第3回光触媒国際シンポジウム
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Metal-oxide-bases photocatalyst for energy and environment2019

    • Author(s)
      M. Miyauchi
    • Organizer
      Tokyo Institute of Technology and Imperial College London's 2nd Workshop on Plastic Electronics
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] TiO2 Based Photocatalyst for Environmental Remediation Using the Concept of Interfacial Charge Transfer Driven by Visible Light2018

    • Author(s)
      M. Miyauchi
    • Organizer
      Energy Materials and Nanotechnology 2018 (EMN 2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Interfacial Charge Transfer between Ultrathin CuOx Film and Rutile TiO2 and Its Application for Efficient Photocatalysis2018

    • Author(s)
      M. Miyauchi
    • Organizer
      22nd International Conference on Photochemical Conversion and Storage of Solar Energy
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 温和な溶液プロセスによるナノクラスター担持光触媒の開発2018

    • Author(s)
      宮内雅浩
    • Organizer
      日本セラミックス協会 第31回秋季シンポジウム
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 環境浄化と人工光合成、それぞれの光触媒の設計2018

    • Author(s)
      宮内雅浩
    • Organizer
      光触媒工業会2018年度技術研究会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Book] 抗菌・抗ウイルス剤の最新動向2021

    • Author(s)
      宮内雅浩
    • Total Pages
      365
    • Publisher
      シーエムシー出版
    • ISBN
      9784781316017
    • Related Report
      2021 Annual Research Report

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Published: 2018-04-23   Modified: 2022-12-28  

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