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2018 Fiscal Year Annual Research Report

Development of photocatalytic CO2 reduction systems using hybrids of carbon nitride semiconductors and metal complexes

Research Project

Project/Area Number 16H06130
Research InstitutionTokyo Institute of Technology

Principal Investigator

前田 和彦  東京工業大学, 理学院, 准教授 (40549234)

Project Period (FY) 2016-04-01 – 2019-03-31
Keywords光触媒 / 金属錯体 / 二酸化炭素固定化 / 半導体 / 人工光合成
Outline of Annual Research Achievements

Ru(II)単核錯体/窒化炭素融合光触媒は、可視光照射下でのCO2のギ酸への還元反応において高いみかけの量子収率、選択率、そして耐久性(触媒回転数)を有する。本年度はこの光触媒に関し、時間分解可視-赤外分光法と発光分光法を用いて光励起キャリアの挙動を調べた。その結果、光励起後に窒化炭素の伝導帯付近に生成した電子が、Ru錯体へ数ピコ秒の速い時間オーダーで移動していることを明らかとした。論文はJ. Phys. Chem. C誌に発表した。尚、本研究は豊田工業大学の山方啓准教授との共同研究成果である。
高いギ酸生成性能とは対照的に、金属錯体/窒化炭素融合光触媒のCO2 → CO変換の効率・耐久性は低く、これらを向上させることが課題となっていた。本年度は、パリ第7大学のMarc Robert教授のグループと共同でFe(II)錯体触媒を組み込んだ窒化炭素融合光触媒系を構築し、CO生成において過去最高となる触媒回転数155、みかけの量子収率4.2%、CO選択率95%以上を達成した。論文はJ. Am. Chem. Soc.誌に発表した。
以上の研究で用いた窒化炭素はバンドギャップが2.7~2.8 eVと比較的大きく、広域可視光の利用という観点では満足なものではない。本年度の研究では、尿素とフェニル尿素の熱重合によって得られる窒化炭素が最大で700 nm程度までの可視光を吸収し、Ru(II)単核錯体と融合することでCO2をギ酸へと変換する光触媒となることを見出した。尿素のみから得た従来型の窒化炭素では反応が進行しなかった500 nm以上の可視光照射下でも、ギ酸を生成することが判明した。論文はACS Sustainable Chem. Eng.誌に発表した。尚、本研究はThe University of New South WalesのRose Amal教授との共同研究成果である。

Research Progress Status

平成30年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

平成30年度が最終年度であるため、記入しない。

  • Research Products

    (23 results)

All 2019 2018 Other

All Int'l Joint Research (2 results) Journal Article (6 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 6 results,  Open Access: 2 results) Presentation (14 results) (of which Int'l Joint Research: 11 results,  Invited: 9 results) Remarks (1 results)

  • [Int'l Joint Research] ニューサウスウェールズ大学(オーストラリア)

    • Country Name
      AUSTRALIA
    • Counterpart Institution
      ニューサウスウェールズ大学
  • [Int'l Joint Research] パリ第7大学(フランス)

    • Country Name
      FRANCE
    • Counterpart Institution
      パリ第7大学
  • [Journal Article] A Visible-Light-Driven Z-Scheme CO2 Reduction System Using Ta3N5 and a Ru(II) Binuclear Complex2019

    • Author(s)
      Kanemichi Muraoka, Tomoki Uchiyama, Daling Lu, Yoshiharu Uchimoto, Osamu Ishitani, Kazuhiko Maeda
    • Journal Title

      Bull. Chem. Soc. Jpn.

      Volume: 92 Pages: 124~126

    • DOI

      10.1246/bcsj.20180239

    • Peer Reviewed / Open Access
  • [Journal Article] Excited-State Dynamics of Graphitic Carbon Nitride Photocatalyst and Ultrafast Electron Injection to a Ru(II) Mononuclear Complex for Carbon Dioxide Reduction2018

    • Author(s)
      Ryo Kuriki, Chandana Sampath Kumara Ranasinghe, Yasuomi Yamazaki, Akira Yamakata, Osamu Ishitani, Kazuhiko Maeda
    • Journal Title

      J. Phys. Chem. C

      Volume: 122 Pages: 16795~16802

    • DOI

      10.1021/acs.jpcc.8b03996

    • Peer Reviewed
  • [Journal Article] Copolymerization Approach to Improving Ru(II)-Complex/C3N4 Hybrid Photocatalysts for Visible-Light CO2 Reduction2018

    • Author(s)
      Constantine Tsounis, Ryo Kuriki, Kengo Shibata, Junie Jhon M. Vequizo, Daling Lu, Akira Yamakata, Osamu Ishitani, Rose Amal, Kazuhiko Maeda
    • Journal Title

      ACS Sustainable Chem. Eng.

      Volume: 6 Pages: 15333~15340

    • DOI

      10.1021/acssuschemeng.8b03782

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Carbon Nitride/Fe Quaterpyridine Catalytic System for Photostimulated CO2-to-CO Conversion with Visible Light2018

    • Author(s)
      Claudio Cometto, Ryo Kuriki, Lingjing Chen, Kazuhiko Maeda, Tai-Chu Lau, Osamu Ishitani, Marc Robert
    • Journal Title

      J. Am. Chem. Soc.

      Volume: 140 Pages: 7437~7440

    • DOI

      10.1021/jacs.8b04007

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Graphitic carbon nitride prepared from urea as a photocatalyst for carbon dioxide reduction under visible light with the aid of a mononuclear Ru(II) complex2018

    • Author(s)
      Kazuhiko Maeda, Daehyeon An, Ryo Kuriki, Daling Lu, Osamu Ishitani
    • Journal Title

      Beilstein J. Org. Chem.

      Volume: 14 Pages: 1806~1812

    • DOI

      10.3762/bjoc.14.153

    • Peer Reviewed / Open Access
  • [Journal Article] Solar Water Oxidation by a Visible-Light-Responsive Tantalum/Nitrogen-Codoped Rutile Titania Anode for Photoelectrochemical Water Splitting and Carbon Dioxide Fixation2018

    • Author(s)
      Akinobu Nakada, Tomoki Uchiyama, Nozomi Kawakami, Shunta Nishioka, Ryutaro Kamata, Hiromu Kumagai, Osamu Ishitani, Yoshiharu Uchimoto, Kazuhiko Maeda
    • Journal Title

      ChemPhotoChem

      Volume: 3 Pages: 37~45

    • DOI

      10.1002/cptc.201800157

    • Peer Reviewed
  • [Presentation] 広域可視光でCO2を還元するRu(II)単核錯体/C3N4ハイブリッド光触媒の開発2019

    • Author(s)
      柴田健吾・栗木亮・石谷治・前田和彦
    • Organizer
      第123回触媒討論会
  • [Presentation] Artificial photosynthetic assembly constructed with metal complexes, nanoparticles and semiconductors2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      The 2018 MRS Spring Meeting
    • Int'l Joint Research / Invited
  • [Presentation] Surface modified semiconductor photocatalysts for carbon dioxide reduction and water oxidation2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      Beilstein Organic Chemistry Symposium 2018
    • Int'l Joint Research / Invited
  • [Presentation] New Heterogeneous Photocatalysts Constructed with Semiconductors, Nanoparticles, and Metal Complexes toward CO2 Reduction and Water Oxidation2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      THERMEC'2018
    • Int'l Joint Research / Invited
  • [Presentation] Mixed-anion solids for solar-to-fuel energy conversion2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      12th International Conference on Ceramic Materials and Components for Energy and Environmental Applications
    • Int'l Joint Research / Invited
  • [Presentation] Chemical approach to artificial photosynthesis using semiconductors, nanoparticles and metal complexes2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      The 2018 International Symposium on Advancement and Prospect of Catalysis Science & Technology
    • Int'l Joint Research / Invited
  • [Presentation] Visible-Light Reduction of Carbon Dioxide on Metal-Complex/Carbon Nitride Hybrid Photocatalysts2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      The 43rd International Conference on Coordination Chemistry
    • Int'l Joint Research / Invited
  • [Presentation] Visible-Light CO2 Reduction Using Hybrid Photocatalysts Constructed with Carbon Nitride and Ru(II) Binuclear Complex2018

    • Author(s)
      Ryo Kuriki, Osamu Ishitani, Kazuhiko Maeda
    • Organizer
      Beilstein Organic Chemistry Symposium 2018
    • Int'l Joint Research
  • [Presentation] Visible-light-driven Z-scheme Photocatalyst Constructed with Carbon Nitride and a Ru(II) Binuclear Complex for CO2 Reduction2018

    • Author(s)
      Ryo Kuriki, Osamu Ishitani, Kazuhiko Maeda
    • Organizer
      International Conference on Ceramic Materials and Components for Energy and Environmental Applications (CMCEE-12)
    • Int'l Joint Research
  • [Presentation] Demonstration of photocatalytic CO2 reduction under visible light using carbon nitride and a binuclear Ru(II) complex2018

    • Author(s)
      Ryo Kuriki, Akira Yamakata, Osamu Ishitani, Kazuhiko Maeda
    • Organizer
      The 8th Tokyo Conference on Advanced Catalytic Science and Technology (TOCAT8)
    • Int'l Joint Research
  • [Presentation] 有機半導体カーボンナイトライドの光励起キャリアダイナミクスと錯体触媒への電子移動過程の観察2018

    • Author(s)
      栗木亮、山方啓、石谷治、前田和彦
    • Organizer
      第37回固体・表面光化学討論会
  • [Presentation] 半導体光触媒を中核とした水の分解・CO2の固定化反応2018

    • Author(s)
      前田和彦
    • Organizer
      京都工芸繊維大学環境科学センター第1回技術セミナー
    • Invited
  • [Presentation] Materials for Artificial Photosynthesis from Mixed-Anion Compounds to Organic Polymers2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      The 3rd International Conference on Emerging Advanced Nanomaterials
    • Int'l Joint Research / Invited
  • [Presentation] Visible-Light CO2 Reduction Using Mixed-Anion Photocatalysts2018

    • Author(s)
      Kazuhiko Maeda
    • Organizer
      1st International Conference on Advanced Chemistry and Catalysis
    • Int'l Joint Research / Invited
  • [Remarks]

    • URL

      http://www.chemistry.titech.ac.jp/~ishitani/member/kmaeda/Home.html

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Published: 2019-12-27  

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