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Clarification of catalytically active structure of crystalline Mo3VOx and its multi-functionalization

Research Project

Project/Area Number 21K14464
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionKanagawa University

Principal Investigator

Ishikawa Satoshi  神奈川大学, 工学部, 助教 (60813350)

Project Period (FY) 2021-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2022: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2021: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Keywords結晶性複合酸化物 / 酸化触媒 / 活性酸素種 / 多元化 / 触媒活性構造 / 結晶性Mo3VOx複合酸化物 / 結晶構造 / 酸化触媒作用
Outline of Research at the Start

結晶性Mo3VOx(C-MoVO)は低級アルカンや不飽和アルデヒド選択酸化反応に極めて高い触媒活性を示す。C-MoVOは構造を保ったまま異種金属元素の導入が可能であり、これにより触媒活性を制御できる。本研究ではC-MoVO上で生じる酸化活性種を明確化し、固体触媒上における酸化作用を分子レベルで明らかにする。また、多元系C-MoVOの結晶構造を保ったまま構造位置選択的金属元素導入や複数金属元素導入を通して、低級アルカン選択酸化反応における触媒作用の高度制御を目指す。

Outline of Final Research Achievements

Oxidation catalysis over crystalline Mo3VOx catalyst (MoVO), one of the promising oxidation catalysts for selective oxidation of alkanes and unsaturated aldehydes, was clarified. In addition, I succeeded to multi-functionalize MoVO by introducing additional elements without altering its crystal structure. The resulting catalyst, MoVWCuO catalyst, showed excellent catalytic properties for the selective oxidation of acrolein. Through the comparison with the industrial catalyst (ill-crystalline Mo-V-W-Cu mixed metal oxide catalyst), I could conclude that MoVWCuO is the true catalytically active structure of the industrial catalyst.

Academic Significance and Societal Importance of the Research Achievements

本研究では低級アルカンや不飽和アルデヒド選択酸化反応に極めて高い酸化触媒活性を示す結晶性Mo3VOx複合酸化物(MoVO)の酸化触媒機能を調べた。高度に組織化された局所構造中で親電子性の活性酸素種が生じ、これが酸化触媒活性種として機能することを明らかにした。高活性酸化触媒の酸化触媒機能を分子レベルで解明したことの学術的意義は極めて高く、今後の酸化触媒設計に広く波及する成果が得られたと確信している。この触媒は化学工業で使用される触媒のモデルとしても用いられる。この触媒の酸化触媒機能が明らかとなったことで、工業触媒合成の設計指針が得られた。社会的に意義深い成果が得られた。

Report

(3 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • Research Products

    (18 results)

All 2023 2022 2021

All Journal Article (4 results) (of which Peer Reviewed: 4 results) Presentation (11 results) (of which Int'l Joint Research: 3 results,  Invited: 4 results) Book (1 results) Patent(Industrial Property Rights) (2 results)

  • [Journal Article] Acid Catalysis over Crystalline Zr3SO9: Role of the Local Structure in Generating Acidity2023

    • Author(s)
      Tao Meilin、Ishikawa Satoshi、Ikeda Takuji、Yasumura Shunsaku、Shimoda Kosuke、Osuga Ryota、Jing Yuan、Toyao Takashi、Shimizu Ken-ichi、Matsuhashi Hiromi、Ueda Wataru
    • Journal Title

      ACS Catalysis

      Volume: 13 Issue: 7 Pages: 4517-4532

    • DOI

      10.1021/acscatal.3c00225

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Oxidation Catalysis over Solid-State Keggin-Type Phosphomolybdic Acid with Oxygen Defects2022

    • Author(s)
      Ishikawa Satoshi、Ikeda Takuji、Koutani Maki、Yasumura Shunsaku、Amakawa Kazuhiko、Shimoda Kosuke、Jing Yuan、Toyao Takashi、Sadakane Masahiro、Shimizu Ken-ichi、Ueda Wataru
    • Journal Title

      Journal of the American Chemical Society

      Volume: 144 Issue: 17 Pages: 7693-7708

    • DOI

      10.1021/jacs.2c00125

    • Related Report
      2022 Annual Research Report 2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] Nb V Mixed Oxide with a Random Assembly of Pentagonal Units: A Catalyst for Oxidative Dehydrogenation of Ethane and Propane2021

    • Author(s)
      K. Shimoda, S. Ishikawa, K. Matsumoto, M. Miyasawa, M. Takebe, Riku Matsumoto, S. Lee, W. Ueda
    • Journal Title

      ChemCatChem

      Volume: 13 Issue: 13 Pages: 3132-3139

    • DOI

      10.1002/cctc.202100463

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] True Catalytically Active Structure in Mo?V-Based Mixed Oxide Catalysts for Selective Oxidation of Acrolein2021

    • Author(s)
      S. Ishikawa, Y. Yamada, N. Kashio, N. Noda, K. Shimoda, M. Hayashi, T. Murayama, W. Ueda
    • Journal Title

      ACS Catal.

      Volume: 11 Issue: 16 Pages: 10294-10307

    • DOI

      10.1021/acscatal.1c01570

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Presentation] The local catalyst structure and oxidation catalysis over crystalline orthorhombic Mo3VOx for selective oxidation of ethane2022

    • Author(s)
      Satoshi Ishikawa, Nagisa Aoki, Kosuke Shimoda, Takashi Kamachi, Wataru Ueda
    • Organizer
      9th TOCAT
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 酸素欠損を有するKeggin型ポリ酸の酸化触媒作用2022

    • Author(s)
      石川 理史・池田 拓史・幸谷 真芸・ 安村 駿作・ 天川 和彦・下田 光祐・Jing Yuan・鳥屋尾 隆・ 定金 正洋・清水 研一・上田 渉
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 酸素欠損を有するKeggin型リンモリブデン酸の酸化触媒作用2022

    • Author(s)
      石川 理史・池田 拓史・幸谷 真芸・ 安村 駿作・ 天川 和彦・下田 光祐・Jing Yuan・鳥屋尾 隆・ 定金 正洋・清水 研一・上田 渉
    • Organizer
      第55回酸化反応討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] ケーススタディ ~ 結晶性複合酸化物触媒 の結晶構造と触媒作用~2022

    • Author(s)
      石川 理史
    • Organizer
      第32回キャラクタリゼーション講習会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Crystalline Zr3SO9 Oxides with Superior Acid Catalytic Property to the Conventional Sulfated Zirconia2022

    • Author(s)
      Meilin Tao・Satoshi Ishikawa・Takuji Ikeda・Shunsaku Yasumura・Yuan Jing・Takashi Toyao・Ken-ichi Shimizu・Hiromi Matsuhashi・Wataru Ueda
    • Organizer
      第131回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 結晶性複合酸化物触媒の 局所的酸素欠陥と酸化触媒作用2022

    • Author(s)
      石川理史
    • Organizer
      第131回触媒討論会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 多元系Mo-V複合酸化物を用いたアクロレイン選択酸化反応における触媒活性構造2021

    • Author(s)
      石川 理史・山田 雄大・樫尾 直樹・下田 光祐・野田 渚紗・上田 渉
    • Organizer
      第69回石油学会研究発表会
    • Related Report
      2021 Research-status Report
  • [Presentation] Structure-Activity Relationship in Crystalline Mo3VOx in Selective Oxidations.2021

    • Author(s)
      Satoshi Ishikawa・Wataru Ueda
    • Organizer
      The Twelfth International Conference on the Science and Technology for Advanced Ceramics
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Local Catalyst Structure of Mixed Metal Oxide for Selective Oxidations.2021

    • Author(s)
      Satoshi Ishikawa・Wataru Ueda
    • Organizer
      12th International Fundamental Science Congress
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 複合酸化物の局所構造で発現する酸化触媒作用2021

    • Author(s)
      石川 理史・上田 渉
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] ピリジンとKeggin型ポリ酸で構成される結晶性(Py)xPMo12Oy触媒の結晶構造解析と選択酸化能2021

    • Author(s)
      石川 理史・池田 拓史・幸谷 真芸・上田 渉
    • Organizer
      第51回石油・石油化学討論会
    • Related Report
      2021 Research-status Report
  • [Book] Crystalline Metal Oxide Catalysts2022

    • Author(s)
      Satoshi Ishikawa, Wataru Ueda
    • Total Pages
      397
    • Publisher
      Springer Nature Singapore
    • ISBN
      9789811950124
    • Related Report
      2022 Annual Research Report
  • [Patent(Industrial Property Rights)] 複合酸化物固体酸触媒、固体酸触媒、それらを用いた化学反応の実行方法、及び複合酸化物固体酸触媒の製造方法2022

    • Inventor(s)
      石川 理史・陶 美林・上田 渉
    • Industrial Property Rights Holder
      神奈川大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2022-062413
    • Filing Date
      2022
    • Related Report
      2022 Annual Research Report
  • [Patent(Industrial Property Rights)] 複合酸化物固体酸触媒、固体酸触媒、それらを用いた化学反応の実行方法、及び複合酸化物固体酸触媒の製造方法2022

    • Inventor(s)
      石川 理史・陶 美林・上田 渉
    • Industrial Property Rights Holder
      神奈川大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2022-062413
    • Filing Date
      2022
    • Related Report
      2021 Research-status Report

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Published: 2021-04-28   Modified: 2024-01-30  

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