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Creation of acid-base paired sites on zeolite catalysts based on spectroscopic approaches

Research Project

Project/Area Number 21K14459
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 (2022)
Tohoku University (2021)

Principal Investigator

Osuga Ryota  北海道大学, 触媒科学研究所, 助教 (30874250)

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: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2021: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000)
KeywordsZeolites / Spectorscopy / Acid-base pair sites / ゼオライト / 酸・塩基協奏型活性点 / Alペアサイト / 位置選択的脱Al処理 / 精密構造解析
Outline of Research at the Start

ゼオライトの有する酸性水酸基と、アルカリ金属カチオンの導入により生成する格子酸素の塩基点を隣接させることで、「酸・塩基協奏型活性点」の創出を目指す。また、目的の活性点創出のため、活性点の性質や位置に関する情報を赤外(IR)、核磁気共鳴(NMR)などの種々の分光法を用いて解析し、得られた情報を合成検討へとフィードバックすることで、精密な活性点デザインを実現する。最終的には、触媒活性を評価することで、酸・塩基協奏作用が種々の触媒反応に及ぼす影響について明らかとする。

Outline of Final Research Achievements

The dealumination of Beta zeolite in cobalt nitrate aqueous solution protected the framework Al species coordinated with Co2+ species (Al pair sites), which gave selectively reduced the number of isolated Al species. The acid-base paired sites were created by the ion exchange for such Al pair-rich beta zeolites. In addition, high-silica CHA-type zeolites were successfully synthesized by aging treatment for the synthetic gel in the presence of seed crystals at room temperature followed by hydrothermal treatment. The obtained CHA-type zeolites showed a long catalytic lifetime for the MTO reaction.

Academic Significance and Societal Importance of the Research Achievements

ゼオライト触媒において、骨格内Al種の量や位置は活性を支配する重要な因子の1つである。本研究では、比較的簡便なポスト処理で位置選択的に骨格内Al種を取り除くことができた。ゼオライトは実際の工業プロセスでも幅広く用いられているため、本手法が汎用的な手法となれば、学術的には勿論のこと工業的にも大きな意義があると言える。また、これまで合成例がなかったAl量のCHA型ゼオライトの合成手法を確立することができた。CHA型ゼオライトは、様々な反応に対してユニークな形状選択性を発現するため、今回合成したハイシリカなCHA型ゼオライトの触媒活性を詳細に検討することで、新たな触媒反応系が発見される可能性がある。

Report

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

    (23 results)

All 2022 2021

All Journal Article (8 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 7 results,  Open Access: 1 results) Presentation (14 results) (of which Int'l Joint Research: 3 results,  Invited: 3 results) Book (1 results)

  • [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 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Improvement of Catalytic Activity of Ce-MFI-Supported Pd Catalysts for Low-Temperature Methane Oxidation by Creation of Concerted Active Sites2022

    • Author(s)
      Osuga Ryota、Neya Atsushi、Yoshida Motohiro、Yabushita Mizuho、Yasuda Shuhei、Maki Sachiko、Kanie Kiyoshi、Yokoi Toshiyuki、Muramatsu Atsushi
    • Journal Title

      Industrial & Engineering Chemistry Research

      Volume: 61 Issue: 27 Pages: 9686-9694

    • DOI

      10.1021/acs.iecr.2c01410

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Fluoride-free synthesis of high-silica CHA-type aluminosilicates by seed-assisted aging treatment for starting gel2022

    • Author(s)
      Osuga Ryota、Yabushita Mizuho、Matsumoto Takeshi、Sawada Masato、Yokoi Toshiyuki、Kanie Kiyoshi、Muramatsu Atsushi
    • Journal Title

      Chemical Communications

      Volume: 58 Issue: 82 Pages: 11583-11586

    • DOI

      10.1039/d2cc04032h

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Development of Hf-containing SBA-15 catalysts with highly dispersed active sites for 1,3-butadiene production from ethanol and acetaldehyde2022

    • Author(s)
      Osuga Ryota、Fang Peixuan、Nishiyama Haruka、Takizawa Koji、Yagihashi Noritoshi、Yokoi Toshiyuki、Kondo Junko N.
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 346 Pages: 112278-112278

    • DOI

      10.1016/j.micromeso.2022.112278

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 活性点位置を制御したRh含有触媒の開発2022

    • Author(s)
      大須賀遼太
    • Journal Title

      触媒

      Volume: 64 Pages: 308-312

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Clarification of acid site location in MSE-type zeolites by spectroscopic approaches combined with catalytic activity: comparison between UZM-35 and MCM-682022

    • Author(s)
      Toyoda Hiroto、Osuga Ryota、Wang Yong、Park Sungsik、Yazawa Koji、Gies Hermann、Gilbert Christopher J.、Yilmaz Bilge、Kelkar C. P.、Yokoi Toshiyuki
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 7 Pages: 4358-4365

    • DOI

      10.1039/d2cp00215a

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Fabrication of <b>AEI</b>-type aluminosilicate catalyst with sheet-like morphology for direct conversion of propene to butenes2021

    • Author(s)
      Osuga Ryota、Takeuchi Takashi、Sawada Masato、Kunitake Yusuke、Matsumoto Takeshi、Yasuda Shuhei、Onozuka Hiroaki、Tsutsuminai Susumu、Kondo Junko N.、Gies Hermann、Yokoi Toshiyuki
    • Journal Title

      Catalysis Science &amp; Technology

      Volume: 11 Issue: 17 Pages: 5839-5848

    • DOI

      10.1039/d1cy00854d

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [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 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 赤外分光法を用いたゼオライトの酸触媒特性評価2022

    • Author(s)
      大須賀遼太
    • Organizer
      第6回ゼオライトセミナー/GSCセミナー
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Synthesis of high-silica CHA-type aluminosilicates by the seed-assisted agong treatment without fluoride media2022

    • Author(s)
      Osuga Ryota
    • Organizer
      4th International Symposium on Porous Materials 2022
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] フッ素を用いないハイシリカCHA型アルミノシリケートの合成とMTO反応活性評価2022

    • Author(s)
      大須賀遼太、藪下瑞帆、松本剛、澤田真人、蟹江澄志、横井俊之、村松淳司
    • Organizer
      第38回ゼオライト研究発表会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Ce含有MFI型ゼオライト担持金属触媒を用いた低温メタン酸化カップリング反応2022

    • Author(s)
      大須賀遼太、根谷温、芳田元洋、藪下瑞帆、保田修平、真木祥千子、蟹江澄志、横井俊之、村松淳司
    • Organizer
      第52回石油・石油化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] フッ素フリー条件下でのハイシリカCHA型ゼオライトの合成とMTO反応用触媒としての応用2022

    • Author(s)
      大須賀遼太、藪下瑞帆、松本剛、蟹江澄志、横井俊之、村松淳司
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Creation of Concerted Active Sites for Improvement of Catalytic Performance of Ce-MFI-Supported Pd Catalysts in Low-Temperature Methane Oxidation2022

    • Author(s)
      Osuga Ryota、Neya Atsushi、Yoshida Motohiro、Yabushita Mizuho、Yasuda Shuhei、Maki Sachiko、Kanie Kiyoshi、Yokoi Toshiyuki、Muramatsu Atsushi
    • Organizer
      ACS Meetings & Expositions Fall 2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] Mechanochemical Synthesis of Fe-Substituted MWW-type Zeolite Catalysts2022

    • Author(s)
      Osuga Ryota、Tanaka Ginpei、Yabushita Mizuho、Ninomiya Kakeru、Maki Sachiko、Nishibori Maiko、Kanie Kiyoshi、Muramatsu Atsushi
    • Organizer
      The 9th Tokyo Conference on Advanced Catalytic Science and Technology
    • Related Report
      2022 Annual Research Report
  • [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, 肖 &#23159;, 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
    • Related Report
      2021 Research-status Report
  • [Presentation] メカノケミカル法によるFe含有10員環細孔ゼオライトの合成と触媒活性評価2021

    • Author(s)
      田中 銀平, 大須賀 遼太, 藪下 瑞帆, 真木 祥千子, 蟹江 澄志, 村松 淳司
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] Synthesis of zeolite catalysts with well-controlled location of catalytic active sites2021

    • Author(s)
      Ryota Osuga
    • Organizer
      The 5th Foresight Symposium on Organic/Inorganic Nanohybrid Platforms for Precision Tumor Imaging and Therapy 2021
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [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
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Synthesis of Fe-containing MWW zeolites via a mechanochemical method and evaluation of catalytic activity2021

    • Author(s)
      Ginpei Tanaka, Ryota Osuga, Mizuho Yabushita, Sachiko Maki, Kiyoshi Kanie, Atsushi Muramatsu
    • Organizer
      The 18th Japan-Korea Symposium on Catalysis
    • Related Report
      2021 Research-status 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, 肖 &#23159;, 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 Research-status Report
  • [Presentation] ハイシリカなCHA型ゼオライトのフッ素フリー合成とMTO反応活性評価2021

    • Author(s)
      大須賀 遼太, 藪下 瑞帆, 松本 剛, 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 Research-status Report
  • [Book] Position Control of Catalytic Elements in Zeolites” in Crystalline Metal Oxide Catalysts2022

    • Author(s)
      Osuga Ryota、Yokoi Toshiyuki
    • Total Pages
      30
    • Publisher
      Springer Soingapore
    • ISBN
      9789811950131
    • Related Report
      2022 Annual Research Report

URL: 

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

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