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Preparation of Arsenic-Containing Ligands and Development of Novel Catalytic Reactions

Research Project

Project/Area Number 17K05803
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Inorganic chemistry
Research InstitutionThe University of Tokyo

Principal Investigator

Tanabe Yoshiaki  東京大学, 大学院工学系研究科(工学部), 研究員 (20384737)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2019: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2018: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2017: ¥2,860,000 (Direct Cost: ¥2,200,000、Indirect Cost: ¥660,000)
Keywords光反応 / フェロセン / サマリウム / 水 / 酸化反応 / ホスフィン / アンモニア / 窒素固定 / フェロセニウム / 触媒反応 / 金属錯体 / ヒ素
Outline of Final Research Achievements

Molybdenum-catalyzed conversion of molecular dinitrogen into ammonia under ambient reaction conditions has been achieved by using a proton source generated in situ from the ruthenium-catalyzed oxidation of water in combination with visible light and a photosensitizer. The preset reaction system is considered as a new model for the nitrogen fixation by photosynthetic bacteria.
In addition, stoichiometric oxidation of phosphines with water and ferrocenium(III) cation as the oxygen atom source and the oxidizing reagent, respectively, was achieved in acetonitrile under visible-light irradiation by using 2,6-lutidine as the proton acceptor. The reaction required light irradiation, under which fluorescence was observed for the acetonitrile solution of the ferrocenium(III) cation.

Academic Significance and Societal Importance of the Research Achievements

水をアンモニア生成反応のプロトン源として触媒的に使う道筋を初めて示した。またフェロセニウムカチオンが水の酸化剤として働くことによりフェロセンが生成するが、フェロセンに代表されるメタロセンは、窒素をアンモニアへと還元する反応の還元剤として働くことが知られており、本研究成果は窒素をアンモニアへと変換する触媒反応構築のための重要な進捗の一つといえる。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Research-status Report
  • 2017 Research-status Report
  • Research Products

    (10 results)

All 2020 2019 2018 2017

All Journal Article (5 results) (of which Peer Reviewed: 4 results) Presentation (4 results) (of which Int'l Joint Research: 2 results) Book (1 results)

  • [Journal Article] Recent advances in catalytic silylation of dinitrogen using transition metal complexes2019

    • Author(s)
      Yoshiaki Tanabe、Yoshiaki Nishibayashi
    • Journal Title

      Coord. Chem. Rev.

      Volume: 389 Pages: 73-93

    • DOI

      10.1016/j.ccr.2019.03.004

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 常温常圧下でアンモニアを合成する新たな手法の開発―窒素ガスと水を原料とする触媒的アンモニア合成法2019

    • Author(s)
      田辺資明、西林仁昭
    • Journal Title

      クリーンエネルギー

      Volume: 28 (10) Pages: 1-10

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Recent Advances in Nitrogen Fixation upon Vanadium Complexes2019

    • Author(s)
      Yoshiaki Tanabe、Yoshiaki Nishibayashi
    • Journal Title

      Coord Chem Rev.

      Volume: 381 Pages: 135-150

    • DOI

      10.1016/j.ccr.2018.11.005

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Phosphine Oxidation with Water and Ferrocenium(III) Cation Induced by Visible-Light Irradiation2018

    • Author(s)
      Yoshiaki Tanabe、Kazunari Nakajima、Yoshiaki Nishibayashi
    • Journal Title

      Chem. Eur. J.

      Volume: 24 Issue: 70 Pages: 18618-18622

    • DOI

      10.1002/chem.201805129

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Catalytic Conversion of Dinitrogen into Ammonia under Ambient Reaction Conditions by Using Proton Source from Water2017

    • Author(s)
      Yoshiaki Tanabe, Kazuya Arashiba, Kazunari Nakajima, and Yoshiaki Nishibayashi
    • Journal Title

      Chemistry an Asian Journal

      Volume: 12 Issue: 19 Pages: 2544-2548

    • DOI

      10.1002/asia.201701067

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Presentation] ピロール骨格PNP型ピンサー配位子を有するモリブデン錯体の合成と反応性2020

    • Author(s)
      田辺資明、関口義也、栗山翔吾、中島一成、西林仁昭
    • Organizer
      日本化学会第100春季年会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Catalytic Conversion of Dinitrogen into Ammonia under Ambient Reaction Conditions by Using Proton Source from Water2018

    • Author(s)
      Yoshiaki Tanabe、Kazuya Arashiba、Kazunari Nakajima、Yoshiaki Nishibayashi
    • Organizer
      28th International Conference on Organometallic Chemistry
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Catalytic Conversion of N2 into NH3 under Ambient Reaction Conditions by Using Proton Source from H2O2018

    • Author(s)
      Yoshiaki Tanabe、Kazuya Arashiba、Kazunari Nakajima、Yoshiaki Nishibayashi
    • Organizer
      43rd International Conference on Coordination Chemistry
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] フェロセニルカチオンを用いた可視光照射下での水の酸化反応2018

    • Author(s)
      田辺 資明, 中島 一成, 西林 仁昭
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Research-status Report
  • [Book] Transition-Metal-Dinitrogen Complexes: Preparation and Reactivity2019

    • Author(s)
      Yoshiaki Nishibayashi(ed)
    • Total Pages
      496
    • Publisher
      Wiley-VCH
    • ISBN
      9783527344253
    • Related Report
      2018 Research-status Report

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Published: 2017-04-28   Modified: 2021-02-19  

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