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Synthesis of Zeolite Catalysts with Highly Active Isolated Heteroatoms through Co-precipitation of Metal Precursors with Anions

Research Project

Project/Area Number 18K14052
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 InstitutionHokkaido University

Principal Investigator

Otomo Ryoichi  北海道大学, 地球環境科学研究院, 准教授 (10776462)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2020: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2019: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2018: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Keywordsゼオライト / フッ素 / ハフニウム / 移動水素化
Outline of Final Research Achievements

In this study, a novel method for post-synthesis of Hf-Beta was developed. Dealuminated zeolite Beta was impregnated with hafnium chloride with ammonium fluoride together, and then calcined at a high temperature to produce zeolite Hf-Beta. The resulting materials showed extremely high activity for the transfer hydrogenation reaction of ketones. Making use of various characterization techniques as well as quantum chemical calculation, the mechanism for the formation of highly active Hf sites was estimated. It was presumed that during impregnation or calcination at low temperature, Hf-F complex species were generated and decomposed by high temperature calcination to form highly active Hf sites in the zeolite framework.

Academic Significance and Societal Importance of the Research Achievements

ヘテロ金属を含むゼオライトを合成する際には,金属源由来のアニオンが共存することがほとんどであるが,共存アニオンが金属種の状態に及ぼす影響は未解明であり,共存アニオンを積極的に利用した合成法はこれまでにほとんどなかった.本研究では,添加フッ素がゼオライト骨格内Hf原子サイトの形成を促進し,活性点が増加するため高活性なHf-Betaが得られることを見出した.これまでに類似の共存アニオンの効果は報告されておらず,メタロシリケートゼオライトの合成に関するまったく新規な知見が得られただけでなく,これまでのフッ素を用いた合成において見過ごされてきた共存フッ素の効果について見直す転機となる可能性もある.

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • 2018 Research-status Report
  • Research Products

    (13 results)

All 2020 2019 2018 Other

All Int'l Joint Research (2 results) Presentation (11 results) (of which Int'l Joint Research: 3 results,  Invited: 2 results)

  • [Int'l Joint Research] Eindhoven University of Technology(オランダ)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] Eindhoven University of Technology(オランダ)

    • Related Report
      2019 Research-status Report
  • [Presentation] 濃厚ゲルを用いたHf-Betaの短時間合成およびそのルイス酸触媒特性2020

    • Author(s)
      中村太一,大友亮一, 神谷裕一
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Short-term synthesis of Hf-Beta zeolite from dense precursor gel2020

    • Author(s)
      Taichi Nakamura, Ryoichi Otomo, Yuichi Kamiya
    • Organizer
      International Symposium on Porous Materials 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Fluoride-mediated synthesis of highly active Hf -Beta for MPV reduction2019

    • Author(s)
      Taichi Nakamura, Ryoichi Otomo, Yuichi Kamiya
    • Organizer
      17th Korea-Japan Symposium on Catalysis
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] フッ素を添加してポスト合成したHf-Betaのルイス酸触媒特性2019

    • Author(s)
      中村太一,大友亮一, 神谷裕一
    • Organizer
      日本化学会北海道支部2019年夏季研究発表会
    • Related Report
      2019 Research-status Report
  • [Presentation] フルフラール類の移動水素化に高活性を示すHf-Betaのポスト合成2019

    • Author(s)
      中村太一,大友亮一, 神谷裕一
    • Organizer
      第124回触媒討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] フッ素を使ったドライゲルコンバージョン法によるHf-Betaの合成とその触媒特性2019

    • Author(s)
      中村太一,大友亮一, 神谷裕一
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Research-status Report
  • [Presentation] ゼオライト上への高活性Hfサイトの形成を促進する添加フッ素の効果2019

    • Author(s)
      大友亮一、中村太一、染谷巧、神谷裕一
    • Organizer
      第123回触媒討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Hf含有ゼオライトベータのフッ素を用いるポスト合成2018

    • Author(s)
      大友亮一、染谷巧、中村太一、神谷裕一
    • Organizer
      石油学会第67回研究発表会
    • Related Report
      2018 Research-status Report
  • [Presentation] Post-synthesis of Hf-Beta zeolite assisted by NH4F: a new insight into the formation of active Lewis acid sites for MPV reduction2018

    • Author(s)
      Otomo Ryoichi, Someya Takumi, Nakamura Taichi, Kamiya Yuichi
    • Organizer
      2018 International Symposium on Advancement and Prospect of Catalysis Science & Technology
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] フッ素を添加してポスト合成したHf-Betaの触媒特性2018

    • Author(s)
      中村太一、染谷巧、大友亮一、神谷裕一
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Research-status Report
  • [Presentation] バイオマス変換を指向した含酸素官能基の自在な変換を可能にする高活性固体酸触媒の開発2018

    • Author(s)
      大友亮一
    • Organizer
      2018年度触媒学会北海道支部北見地区講演会
    • Related Report
      2018 Research-status Report
    • Invited

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Published: 2018-04-23   Modified: 2022-01-27  

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