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Efficient formose reactions using carbon-based materials as both reaction fields and catalysts

Research Project

Project/Area Number 19K15355
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 InstitutionTohoku University

Principal Investigator

Yabushita Mizuho  東北大学, 工学研究科, 助教 (00835142)

Project Period (FY) 2019-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2021: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2020: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2019: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Keywords炭素材料 / 反応場 / 吸着 / バイオマス / ホルモース反応 / 不均一系触媒 / 塩基触媒 / 窒素ドープ炭素 / 金属有機構造体 / 分子間反応
Outline of Research at the Start

分子間反応の速度は、活性化エネルギーだけでなく、分子同士の出会いやすさ(頻度因子)にも影響を受ける。本研究では、分子間反応として五炭糖とホルムアルデヒドによるホルモース反応に着目し、塩基点を直接導入、あるいは表面に担持した炭素材料を触媒に用いて、六炭糖の高収率合成を目指す。本触媒は、単なる固体塩基触媒として用いるのではなく、糖化合物に対する炭素材料の高い親和性に着目し、基質分子同士が出会い、反応する場として利活用することで、分子間反応であるホルモース反応の高効率化実現を目指す。

Outline of Final Research Achievements

Carbon-based catalysts that originally possess hydrophobic surface for adsorbing both substrates (carbohydrates and formaldehyde) and base sites as active sites were tried to be developed for highly-efficient catalytic systems for formose reactions. For this objective, the nitrogen-doped carbons, in which nitrogen-containing functional groups are assumed to act as active sites due to their basicity, were prepared via the carbonization of porphyrin under various conditions, but they did not exhibit catalytic performance for formose reactions. Another approach to loading metal oxides onto the surface of activated carbon in order to form base sites that show stronger basicity than nitrogen-containing functional groups, base metal oxides was not effective.
Meanwhile, the knowledge about the competitive adsorption processes in the presence of multiple solutes and the modification of metal nanoparticles by metal-oxide clusters has been obtained.

Academic Significance and Societal Importance of the Research Achievements

複数の有機化合物が共存する水溶液中における競争吸着過程、特に木質バイオマスの前処理(有用成分の抽出・反応性向上)に用いられるイオン液体が存在する条件での知見が得られた。これは、今後2050年カーボンニュートラル実現に欠かせない「バイオマス利用」に寄与するものと期待している。また、固体表面のナノ粒子と金属酸化物クラスターを複合化させる触媒の開発に成功し、今後の固体触媒の精密設計に繋がると考えている。

Report

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

    (25 results)

All 2022 2021 2020 2019 Other

All Int'l Joint Research (2 results) Journal Article (7 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 6 results,  Open Access: 1 results) Presentation (16 results) (of which Int'l Joint Research: 6 results,  Invited: 5 results)

  • [Int'l Joint Research] 北京科学技術大学(中国)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] University of California, Berkeley/Northwestern University/Joint BioEnergy Institute(米国)

    • Related Report
      2019 Research-status Report
  • [Journal Article] Development of Synthetic Route for Fe-substituted MWW-type Zeolites Using Mechanochemical Method2022

    • Author(s)
      Osuga Ryota、Tanaka Ginpei、Yabushita Mizuho、Ninomiya Kakeru、Maki Sachiko、Nishibori Maiko、Kanie Kiyoshi、Muramatsu Atsushi
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 65 Issue: 2 Pages: 67-77

    • DOI

      10.1627/jpi.65.67

    • NAID

      130008166207

    • ISSN
      1346-8804, 1349-273X
    • Year and Date
      2022-03-01
    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Deoxydehydration of Biomass‐Derived Polyols Over Silver‐Modified Ceria‐Supported Rhenium Catalyst with Molecular Hydrogen2022

    • Author(s)
      Yamaguchi Kosuke、Cao Ji、Betchaku Mii、Nakagawa Yoshinao、Tamura Masazumi、Nakayama Akira、Yabushita Mizuho、Tomishige Keiichi
    • Journal Title

      ChemSusChem

      Volume: In press Issue: 10

    • DOI

      10.1002/cssc.202102663

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 金属有機構造体NU-1000を用いたバイオマス由来糖化合物と芳香族化合物の選択吸着・分離2022

    • Author(s)
      藪下瑞帆、福岡淳
    • Journal Title

      月刊ファインケミカル

      Volume: 4

    • NAID

      130007778070

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Adsorption of Keggin-Type Polyoxometalates on Rh Metal Particles under Reductive Conditions2021

    • Author(s)
      Nakagawa Yoshinao、Kuwata Ayaka、Yamaguchi Kosuke、Tamura Masazumi、Yabushita Mizuho、Tomishige Keiichi
    • Journal Title

      Inorganic Chemistry

      Volume: 60 Issue: 16 Pages: 12413-12424

    • DOI

      10.1021/acs.inorgchem.1c01644

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Transcription-induced formation of paired Al sites in high-silica CHA-type zeolite framework using Al-rich amorphous aluminosilicate2021

    • Author(s)
      Yabushita Mizuho、Imanishi Yoshiyasu、Xiao Ting、Osuga Ryota、Nishitoba Toshiki、Maki Sachiko、Kanie Kiyoshi、Cao Wenbin、Yokoi Toshiyuki、Muramatsu Atsushi
    • Journal Title

      Chemical Communications

      Volume: 57 Issue: 98 Pages: 13301-13304

    • DOI

      10.1039/d1cc05401e

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Selective Separation of Biomass-Derived Sugars and Aromatics with Aromatic Domains of Metal-Organic Frameworks and Surface-Modified Silica2020

    • Author(s)
      Mizuho Yabushita, Atsushi Fukuoka
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: -

    • NAID

      130007868036

    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Journal Article] Effect of ionic liquid on sugar-aromatic separation selectivity by metal-organic framework NU-1000 in aqueous solution2019

    • Author(s)
      Mizuho Yabushita, Gabriella Papa, Peng Li, Atsushi Fukuoka, Omar K. Farha, Blake A. Simmons, Alexander Katz
    • Journal Title

      Fuel Processing Technology

      Volume: 197 Pages: 106189-106189

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Transcription-induced formation of Al pair sites in CHA-type aluminosilicate using Al-rich amorphous aluminosilicate precursor2022

    • Author(s)
      Yoshiyasu Imanishi, Ting Xiao, Mizuho Yabushita, Ryota Osuga, Toshiki Nishitoba, Sachiko Maki, Kiyoshi Kanie, Wenbin Cao, Toshiyuki Yokoi, Atsushi Muramatsu
    • Organizer
      The 9th Tokyo Conference on Advanced Catalytic Science and Technology
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Ce含有MFI型ゼオライト担持パラジウム触媒による低温メタン酸化カップリング反応2021

    • Author(s)
      藪下 瑞帆, 芳田 元洋, 大須賀 遼太, 武藤 郁弥, 井口 翔之, 保田 修平, 根谷 温, 堀江 真未, 真木 祥千子, 蟹江 澄志, 山中 一郎, 横井 俊之, 村松 淳司
    • Organizer
      第51回石油・石油化学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 非晶質メタロシリケートを前駆体に用いたヘテロ元素含有ゼオライトの合成とその応用2021

    • Author(s)
      藪下 瑞帆
    • Organizer
      2021年度石油学会ジュニア・ソサイアティ(JPIJS)討論会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Heteroatom-containing zeolite catalysts prepared from amorphous metallosilicates for oxidative conversion of methane2021

    • Author(s)
      Mizuho Yabushita
    • Organizer
      The 9th Workshop on Next-Generation Utilization of Natural Gas
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] CHA型ゼオライト中の骨格内Al原子分布の制御とイオン交換能の評価2021

    • Author(s)
      今西 佳保, Xiao Ting, 大須賀 遼太, 藪下 瑞帆, 真木 祥千子, 蟹江 澄志, 横井 俊之, 村松 淳司
    • Organizer
      石油学会 第63回年会(第69回研究発表会)
    • Related Report
      2021 Annual Research Report
  • [Presentation] Ag修飾CeO2担持ReOx触媒を用いたエリスリトールから1,3-ブタジエンへの脱酸素脱水(DODH)反応2021

    • Author(s)
      山口 功祐, 中川 善直, 藪下 瑞帆, 冨重 圭一
    • Organizer
      第41回触媒学会若手会「夏の研修会」
    • Related Report
      2021 Annual Research Report
  • [Presentation] 銀修飾セリア担持レニウム触媒を用いたエリスリトールから1,3-ブタジエンへの脱酸素脱水反応2021

    • Author(s)
      山口 功祐, 中川 善直, 田村 正純, 藪下 瑞帆, 冨重 圭一
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Synthesis of Fe-substituted MWW-type zeolites via a mechanochemical method2021

    • Author(s)
      Ginpei Tanaka, Ryota Osuga, Mizuho Yabushita, Kakeru Ninomiya, Sachiko Maki, Maiko Nishibori, Kiyoshi Kanie, Atsushi Muramatsu
    • Organizer
      International Symposium on Porous Materials 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Deoxydehydration of Biomass-derived Polyols over ReOx-Ag/CeO2 catalyst with Molecular Hydrogen2021

    • Author(s)
      Kosuke Yamaguchi, Ji Cao, Yoshinao Nakagawa, Masazumi Tamura, Mizuho Yabushita, Keiichi Tomishige
    • Organizer
      The 18th Japan-Korea Symposium on Catalysis
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis of CHA-type zeolites with paired Al sites using Al-rich amorphous aluminosilicate2021

    • Author(s)
      Yoshiyasu Imanishi, Ting Xiao, Mizuho Yabushita, Ryota Osuga, Toshiki Nishitoba, Sachiko Maki, Kiyoshi Kanie, Wenbin Cao, Toshiyuki Yokoi, Atsushi Muramatsu
    • Organizer
      2021Annual Joint Symposium Tohoku University & National Taipei University of Technology: Exploration - Expansion - Acceleration
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Alペアサイトを有するCHA型ゼオライトの合成とイオン交換特性評価2021

    • Author(s)
      今西 佳保, Xiao Ting, 大須賀 遼太, 藪下 瑞帆, 真木 祥千子, 蟹江 澄志, 横井 俊之, 村松 淳司
    • Organizer
      第37回ゼオライト研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Deoxydehydration of erythritol to butadiene over ceria-supported rhenium catalysts modified with metals2021

    • Author(s)
      Kosuke Yamaguchi, Yoshinao Nakagawa, Masazumi Tamura, Mizuho Yabushita, Keiichi Tomishige
    • Organizer
      The International Chemical Congress of Pacific Basin Societies 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Selective Separation of Biomass-Derived Sugars and Aromatics with Aromatic Domains of Well-Designed Materials2020

    • Author(s)
      藪下 瑞帆
    • Organizer
      令和2年度化学系学協会東北大会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] 触媒としての炭素材料の利活用:炭素材料を用いた非可食バイオマスの分解反応2019

    • Author(s)
      藪下瑞帆
    • Organizer
      第57回炭素材料夏季セミナー
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] メカノケミカル反応を活用した金属骨格置換ゼオライトの合成とメタン転換活性評価2019

    • Author(s)
      藪下瑞帆
    • Organizer
      第19回石油学会北海道支部講演会
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] Selective separation of biomass-derived sugars and aromatics with metal-organic framework NU-10002019

    • Author(s)
      Mizuho Yabushita, Atsushi Fukuoka, Omar K. Farha, Alexander Katz
    • Organizer
      第49回石油・石油化学討論会
    • Related Report
      2019 Research-status Report

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

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