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Metal-free and heterogeneous catalysts

Research Project

Project/Area Number 19H02718
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 33020:Synthetic organic chemistry-related
Research InstitutionOkayama University

Principal Investigator

Nishina Yuta  岡山大学, 異分野融合先端研究コア, 研究教授 (50585940)

Project Period (FY) 2019-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥17,160,000 (Direct Cost: ¥13,200,000、Indirect Cost: ¥3,960,000)
Fiscal Year 2021: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Fiscal Year 2020: ¥6,500,000 (Direct Cost: ¥5,000,000、Indirect Cost: ¥1,500,000)
Fiscal Year 2019: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Keywordsカーボン / 触媒 / 化学修飾 / 電子移動 / 酸化還元 / メタルフリー / グラフェン / 有機合成 / ラジカル / カーボン触媒 / 水素化 / カップリング
Outline of Research at the Start

カーボンを触媒として利用する有機合成反応の開発は,2010年頃に研究が展開された新しい分野である。そのため,反応メカニズムや活性点に関して未解明な点が多く,カーボン触媒の開発は試行錯誤に頼っているのが現状である。本研究では,カーボンやそのモデルとなる低分子に対して化学修飾により官能基やラジカルを付与して触媒性能を評価することにより,触媒活性が発現するメカニズムを解明する。とくに,官能基やラジカルを有する多環芳香族化合物をカーボン触媒のモデルとして合成し,その触媒性能を評価することは新規性・学術性ともに高く,これまでブラックボックスであったカーボン触媒の真相を明らかにする。

Outline of Final Research Achievements

Aiming to build the concept of "carbon catalyst" that does not rely on metal species, this research confirmed the reactivity of carbon materials by changing their structure and functional groups. Through this research, it was found that incorporating nitrogen atoms into carbon and increasing radicals are effective for catalytic activity. It was also found that it is possible to increase radicals by cleaving oxygen functional groups on the carbon surface. It was clarified that nitrogen-doped carbon can be used as a catalyst for the reduction of nitro groups and reduction of oxygen molecules. The carbon material was also found to be effective for the polymerization of styrene, acrylonitrile, vinylpyridine, and styrene sulfonic acid. The detailed mechanism was analyzed by in situ ESR spectroscopy.

Academic Significance and Societal Importance of the Research Achievements

カーボン触媒は世界的に研究が盛んになってきているにも関わらず,触媒科学としての基礎的な検討が欠けていると感じている。そこで申請者は,カーボンの組成を系統的にコントロールし,化学修飾によりナノ~原子・分子レベルで構造を変え,in situ分析などを通して触媒活性が発現するメカニズムを解明(場合によっては過去の研究事例を否定)するとともに,高活性化・高選択性の発現・新反応の開拓を実現するためのカーボン触媒の設計指針を確立することが重要であるとの考えに至った。なぜカーボンが,金属触媒に似た反応や異なる選択性を示すのかを明らかにすることが,本研究の意義である。

Report

(4 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • Research Products

    (15 results)

All 2022 2021 2020 2019 Other

All Int'l Joint Research (3 results) Journal Article (8 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 8 results,  Open Access: 2 results) Presentation (3 results) (of which Int'l Joint Research: 1 results,  Invited: 3 results) Remarks (1 results)

  • [Int'l Joint Research] Univ. Grenoble Alpes(フランス)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] CMRDI(エジプト)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] Rutgers University(米国)

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Grafting redox-active molecules on graphene oxide through diamine linker: the length optimization for electron transfer2022

    • Author(s)
      R. Khan, Y. Nishina
    • Journal Title

      Dalton Trans

      Volume: 51 Issue: 5 Pages: 1874-1874

    • DOI

      10.1039/d1dt03197j

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Bottom-up synthesis of nitrogen-doped nanocarbons by a combination of metal catalysis and a solution plasma process2020

    • Author(s)
      Y. Zhou, Y. Nishina
    • Journal Title

      Nanoscale Adv.

      Volume: 2 Issue: 10 Pages: 4417-4417

    • DOI

      10.1039/d0na00327a

    • NAID

      120007004830

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Unveiling the Mechanism of Polymer Grafting on Graphene for Functional Composites: The Behavior of Radicals2020

    • Author(s)
      Y. Hori, K. Kubo, Y. Nishina
    • Journal Title

      Macromol. Rapid Commun.

      Volume: - Issue: 8 Pages: 2000577-2000577

    • DOI

      10.1002/marc.202000577

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Graphene-based carbocatalysts for carbon-carbon bond formation2020

    • Author(s)
      M. S. Ahmad, Y. Nishina
    • Journal Title

      Nanoscale

      Volume: 12 Issue: 23 Pages: 12210-12227

    • DOI

      10.1039/d0nr02984j

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Simple and Robust Functionalization of Graphene for Advanced Energy Devices2020

    • Author(s)
      R. Khan, R. Nakagawa, B. Campeon, Y. Nishina
    • Journal Title

      ACS Appl. Mater. Interfaces

      Volume: 12 Issue: 11 Pages: 12736-12742

    • DOI

      10.1021/acsami.9b21082

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Dehydrogenative Coupling of Toluene Promoted by Multi-Walled Carbon Nanotubes2020

    • Author(s)
      El-Hout, S. I.; Zhou, Y.; Kano, J.; Uchida, Y.; Nishina, Y.
    • Journal Title

      Catal Lett

      Volume: 150 Issue: 1 Pages: 256-262

    • DOI

      10.1007/s10562-019-02951-z

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Electrosynthesis of Pyrenediones on Carbon Nanotube Electrodes for Efficient Electron Transfer with FAD‐dependent Glucose Dehydrogenase in Biofuel Cell Anodes2019

    • Author(s)
      Pierre‐Yves Blanchard, Paulo Henrique M. Buzzetti, Bridget Davies, Yannig Nedellec, Emerson Marcelo Girotto, Andrew J. Gross, Alan Le Goff, Yuta Nishina, Serge Cosnier, Michael Holzinger
    • Journal Title

      ChemElectroChem

      Volume: 6 Issue: 20 Pages: 5242-5247

    • DOI

      10.1002/celc.201901666

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Selective Hydrogenation by Carbocatalyst: The Role of Radicals2019

    • Author(s)
      Muhammad Sohail Ahmad, Huixin He, Yuta Nishina
    • Journal Title

      Org. Lett.

      Volume: 21 Issue: 20 Pages: 8164-8168

    • DOI

      10.1021/acs.orglett.9b02432

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 機能性炭素素材をベンチャービジネスに!酸化グラフェンの産業化2021

    • Author(s)
      仁科勇太
    • Organizer
      第11回CSJ化学フェスタ
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] グラフェン材料の開発と応用展開2021

    • Author(s)
      仁科勇太
    • Organizer
      グラフェンコンソーシアム 第27回研究講演会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Metal-free Carbocatalysts for Hydrogenation Reactions2021

    • Author(s)
      Yuta Nishina
    • Organizer
      PACIFICHEM 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Remarks] 機能分子工学研究室

    • URL

      http://www.tt.vbl.okayama-u.ac.jp/

    • Related Report
      2019 Annual Research Report

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Published: 2019-04-18   Modified: 2023-01-30  

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