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Development of a new zeolite synthesis method that dramatically expands the possibility of creating high-performance catalysts

Research Project

Project/Area Number 19H02513
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionYokohama National University

Principal Investigator

Kubota Yoshihiro  横浜国立大学, 大学院工学研究院, 教授 (30283279)

Co-Investigator(Kenkyū-buntansha) 池田 拓史  国立研究開発法人産業技術総合研究所, 材料・化学領域, 上級主任研究員 (60371019)
Project Period (FY) 2019-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2021: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2020: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2019: ¥7,410,000 (Direct Cost: ¥5,700,000、Indirect Cost: ¥1,710,000)
Keywords新型ゼオライト / 合成 / 構造解析 / 高性能触媒 / ゼオライト触媒
Outline of Research at the Start

(1) ゼオライトの骨格構造を制御する,(2) 活性点の位置や分布を微視的な観点から制御する,(3) 巨視的な観点から,粒子の階層構造を作り込む。(1) は,斬新な合成法の開発を経て自ら新規ゼオライトを創出することを含む。得られた新型ゼオライトにつき (2)と(3)を検討し,高活性・高選択性・高耐久性(長寿命)を併せもつゼオライト触媒の,従来よりも簡便で汎用性の高い調製法を開発する。そして,酸触媒・酸化触媒活性点の付与により,省エネルギー型・環境調和型の触媒化学プロセスを構築することを最終目標とする。この過程で,ゼオライトの精密分析手法の進化も図る。

Outline of Final Research Achievements

The ultimate goal of this task is to provide a preparation technique of zeolite catalyst that can be readily utilized in general, and to contribute not only to basic research but also to the acceleration of catalyst development and social implementation that are closer to industrial applications. In this connection, hierarchical structure was successfully created in YNU-5 zeolite by a direct base-treatment. The mesopore/micropore hierarchical structure in the YNU-5 zeolite catalyst suppressed deactivation more than the non-hierarchical, dealuminated YNU-5 with a similar Si/Al ratio.

Academic Significance and Societal Importance of the Research Achievements

新規骨格をもつYNU-5ゼオライト触媒の高性能化へのアプローチとして,ごく普通の塩基処理とそれに続く酸処理によって,有効な酸点を保持しつつ粒子内の拡散性を向上させうる階層構造を導入できたことは,本触媒の実用化へ向けても有意義なことである。YNU-5の特異なYFI骨格に由来する強い酸点について,学術的にも興味深い事実が最近見つかっており,今後の展開が期待できる。また,YNU-5の合成のために複雑な構造規定剤を有機合成する必要は無く,再現性も比較的高いことは,社会実装へ向けて有利な要素と言える。以上より,本研究成果の学術的意義や社会的意義は大きい。

Report

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

    (57 results)

All 2022 2021 2020 2019 Other

All Int'l Joint Research (2 results) Journal Article (11 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 11 results,  Open Access: 4 results) Presentation (42 results) (of which Int'l Joint Research: 11 results,  Invited: 2 results) Remarks (1 results) Patent(Industrial Property Rights) (1 results)

  • [Int'l Joint Research] ENSICAEN(フランス)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] University of Sofia(ブルガリア)

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Acidic property of YNU-5 zeolite influenced by its unique micropore system2022

    • Author(s)
      Katada Naonobu、Yamamoto Kana、Fukui Moeri、Asanuma Kai、Inagaki Satoshi、Nakajima Kazuki、Suganuma Satoshi、Tsuji Etsushi、Palcic Ana、Valtchev Valentin、Petkov Petko St.、Simeonova Kristina、Vayssilov Georgi N.、Kubota Yoshihiro
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 330 Pages: 111592-111592

    • DOI

      10.1016/j.micromeso.2021.111592

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] GAM-4: a novel microporous silicoaluminophosphate crystal formed by the interzeolite conversion of SAPO-5 zeolite2022

    • Author(s)
      Komura Kenichi、Aoki Hisakazu、Ikeda Takuji
    • Journal Title

      Journal of Porous Materials

      Volume: 29 Issue: 2 Pages: 583-590

    • DOI

      10.1007/s10934-021-01183-0

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Introduction of Hierarchical Structure into YNU-5 Zeolite and Its Enhanced Catalytic Performance for Hexane Cracking2021

    • Author(s)
      Liu Qing、Sugimoto Ryota、Inagaki Satoshi、Kubota Yoshihiro
    • Journal Title

      Chemistry Letters

      Volume: 50 Issue: 9 Pages: 1725-1728

    • DOI

      10.1246/cl.210368

    • NAID

      130008088226

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Defect Formation, T-Atom Substitution and Adsorption of Guest Molecules in MSE-Type Zeolite Framework?DFT Modeling2021

    • Author(s)
      Petkov Petko St.、Simeonova Kristina、Koleva Iskra Z.、Aleksandrov Hristiyan A.、Kubota Yoshihiro、Inagaki Satoshi、Valtchev Valentin、Vayssilov Georgi N.
    • Journal Title

      Molecules

      Volume: 26 Issue: 23 Pages: 7296-7296

    • DOI

      10.3390/molecules26237296

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Multiple templating strategy for the control of aluminum and phosphorus distributions in AFX zeolite2021

    • Author(s)
      Tsunoji Nao、Tsuchiya Kazuyoshi、Nakazawa Naoto、Inagaki Satoshi、Kubota Yoshihiro、Nishitoba Toshiki、Yokoi Toshiyuki、Ohnishi Takeshi、Ogura Masaru、Sadakane Masahiro、Sano Tsuneji
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 321 Pages: 111124-111124

    • DOI

      10.1016/j.micromeso.2021.111124

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Unveiling unique structural features of the YNU-5 aluminosilicate family2021

    • Author(s)
      Zhang Yaping、Zhou Yi、Sun Tu、Chen Pengyu、Li Chengmin、Kubota Yoshihiro、Inagaki Satoshi、Dejoie Catherine、Mayoral Alvaro、Terasaki Osamu
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 317 Pages: 110980-110980

    • DOI

      10.1016/j.micromeso.2021.110980

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Highly efficient titanosilicate catalyst Ti-MCM-68 prepared using liquid-phase titanium source for the phenol oxidation2021

    • Author(s)
      S. Inagaki, R. Ishizuka, Y. Ikehara, S. Odagawa, K. Asanuma, S. Morimoto, Y. Kubota
    • Journal Title

      RSC Advances

      Volume: 11 Issue: 6 Pages: 3681-3684

    • DOI

      10.1039/d0ra10081a

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] The synthesis of YNU-5 zeolite and its application to the catalysis in the dimethyl ether-to-olefin reaction2020

    • Author(s)
      Q. Liu, Y. Yoshida, N. Nakazawa, S. Inagaki, Y. Kubota
    • Journal Title

      Materials

      Volume: 13 Issue: 9 Pages: 2030-2044

    • DOI

      10.3390/ma13092030

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Solid-state NMR and powder X-ray diffraction studies on ammonium ion-exchanged and dealuminated zeolite YNU-52020

    • Author(s)
      Ikeda Takuji、Yoshida Yuka、Nakazawa Naoto、Inagaki Satoshi、Kubota Yoshihiro
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 302 Pages: 110197-110197

    • DOI

      10.1016/j.micromeso.2020.110197

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of a new zeolite YNU-5 and stabilization of its framework toward catalytic application2019

    • Author(s)
      窪田好浩,稲垣怜史,中澤直人
    • Journal Title

      ゼオライト

      Volume: 36 Issue: 4 Pages: 115-124

    • DOI

      10.20731/zeoraito.36.4.115

    • NAID

      40022052918

    • ISSN
      0918-7774
    • Year and Date
      2019-10-15
    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of novel aluminosilicate YNU-5 and enhancement of the framework thermal stability by post-synthesis treatment2019

    • Author(s)
      N. Nakazawa, Y. Yoshida, S. Inagaki, Y. Kubota
    • Journal Title

      Microporous Mesoporous Materials

      Volume: 280 Pages: 66-74

    • DOI

      10.1016/j.micromeso.2019.01.004

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Presentation] Preparation and Catalytic Properties of Novel Titanosilicate with YFI-type Framework2021

    • Author(s)
      Yoshihiro Kubota
    • Organizer
      FEZA2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Highly efficient titanosilicate catalyst Ti-MCM-68 for the oxidation of phenol with hydrogen peroxide2021

    • Author(s)
      Satoshi Inagaki
    • Organizer
      FEZA2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 脱AlしたYNU-5の固体酸触媒としての応用2021

    • Author(s)
      杉本遼太
    • Organizer
      第37回ゼオライト研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 8員環ゼオライトのスチーミングによる脱Al挙動2021

    • Author(s)
      奥田多絵
    • Organizer
      第37回ゼオライト研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Selective oxidation over FAU-type titanosilicate prepared by vapor phase TiCl4 treatment2021

    • Author(s)
      張 聖翔
    • Organizer
      第37回ゼオライト研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 液相Ti導入したTi-MCM-68の活性点構造解明へ向けた紫外・可視分光法によるアプローチ2021

    • Author(s)
      小田川翔大
    • Organizer
      第37回ゼオライト研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Synthesis and framework stabilization of YNU-5 zeolite for catalytic application2021

    • Author(s)
      Yoshihiro Kubota
    • Organizer
      International Symposium on Materials of the Millennium: Emerging Trends and Future Prospects (MMETFP-2021)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] YNU-5ゼオライトへの階層構造の導入とヘキサンの接触分解に対する触媒性能の向上2021

    • Author(s)
      窪田好浩
    • Organizer
      第51回石油・石化討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 第四級アンモニウムTEBOP2+誘導体を構造規定剤とするAFX型ゼオライトの合成2021

    • Author(s)
      奥田多絵
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] TiCl4加水分解物を用いた簡便な調製法で得られたTi-MCM-68の触媒特性2021

    • Author(s)
      小田川翔大
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Preparation of hierarchical YNU-5 zeolite through alkaline leaching2020

    • Author(s)
      Q. Liu, S. Inagaki, Y. Kubota
    • Organizer
      Japan-India YNU Symposium 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 脱AlしたYNU-5の固体酸触媒特性2020

    • Author(s)
      杉本遼太,淺沼 開,稲垣怜史,窪田好浩
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] YFI型チタノシリケートの調製過程における脱Al処理条件の検討2020

    • Author(s)
      淺沼開,稲垣怜史,窪田好浩
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] MSE型ゼオライトの酸処理による脱Alと骨格構造の安定化2020

    • Author(s)
      大類有基,難波晃史,稲垣怜史,窪田好浩
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 脱アルミニウムYNU-5ゼオライトの酸性質2020

    • Author(s)
      福井萌麗,山本花菜,森脇 優,淺沼 開,稲垣怜史,窪田好浩,辻 悦司,菅沼学史,片田直伸
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Ti-betaを触媒とするフェノールの酸化での選択性の制御2020

    • Author(s)
      稲垣怜史,淺沼開,横瀬結友,窪田好浩
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 種々の液相処理法でTi導入したTi-MCM-68の調製2020

    • Author(s)
      小田川翔大,石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第36回ゼオライト研究発表会
    • Related Report
      2020 Annual Research Report
  • [Presentation] Cosolvent Effect on Selectivity in the Phenol Oxidation with H2O2 over Ti-beta Catalyst2020

    • Author(s)
      S. Inagaki, M. Takeyama, K. Asanuma, Y. Yokose, Y. Kubota
    • Organizer
      International Symposium on Porous Materials 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 脱AlしたMCM-68の簡便なTiCl4水溶液処理による高性能Ti-MCM-68触媒の調製2020

    • Author(s)
      小田川翔大,石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] YFI型チタノシリケートの酸化触媒性能2020

    • Author(s)
      淺沼 開,稲垣怜史,窪田好浩
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] YNU-5ゼオライトの大細孔からアクセス可能な強ブレンステッド酸点2020

    • Author(s)
      山本花菜,淺沼 開,稲垣怜史,窪田好浩
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] YFI型ゼオライトの合成および固体酸触媒としての応用2020

    • Author(s)
      杉本遼太,淺沼 開,稲垣怜史,窪田好浩
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 固体NMRにおけるAFX型ゼオライトの活性点分布の解析2020

    • Author(s)
      稲垣怜史,杉本遼太,大類有基,難波晃史,石塚 遼,中澤直人,窪田好浩
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 新規骨格チタノシリケートTi-YNU-5の調製と選択酸化触媒としての応用2019

    • Author(s)
      淺沼 開,石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] MSE型ゼオライトの液相Ti修飾とフェノール酸化触媒としての応用2019

    • Author(s)
      石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] MSE型アルミノシリケートの二段階酸処理による骨格構造の安定化と脱Al2019

    • Author(s)
      難波晃史,韓 喬,稲垣怜史,窪田好浩
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] ケージ型細孔を持つゼオライトの細孔分布解析2019

    • Author(s)
      重岡俊裕, 船橋太一, 仲井和之, 田中秀樹, 宮原 稔, 稲垣怜史, 窪田好浩
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] YFI型ゼオライトの酸性質2019

    • Author(s)
      山本花菜,窪田好浩,稲垣怜史,淺沼 開,中島一樹,中村浩史郎,菅沼学史,辻悦司,片田直伸
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] かさ高く剛直な有機構造規定剤を用いたリン修飾AFXゼオライトの合成2019

    • Author(s)
      土谷和愛,津野地直,中澤直人,窪田好浩,西鳥羽俊貴,横井俊之,大西武士,小倉賢,佐野庸治
    • Organizer
      第35回ゼオライト研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Effect of phase purity of YNU-5 catalyst on dimethyl ether-to-olefin reaction2019

    • Author(s)
      Q. Liu, Y. Yoshida, N. Nakazawa, S. Inagaki, Y. Kubota
    • Organizer
      International Symposium on Porous Materials 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Ceria-modified MCM-68 as an efficient catalyst for the production oflight olefins2019

    • Author(s)
      Q. Han, K. Enoeda, S. Inagaki, Y. Kubota
    • Organizer
      International Symposium on Porous Materials 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ケージ型細孔を持つゼオライトの細孔分布解析2019

    • Author(s)
      重岡俊裕, 船橋太一, 仲井和之, 田中秀樹, 宮原 稔, 稲垣怜史, 窪田好浩
    • Organizer
      第33回日本吸着学会研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 新型チタノシリケートの創製と酸化触媒性能2019

    • Author(s)
      窪田好浩,稲垣怜史,石塚 遼,淺沼 開
    • Organizer
      第49回石油・石化討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Synthesis and framework stabilization of new zeolite YNU-5 for catalytic application2019

    • Author(s)
      Y. Kubota, N. Nakazawa, Y. Yoshida, S. Inagaki
    • Organizer
      2019 International Conference on Nanospace Materials (ICNM 2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 液相Ti修飾処理によるMSE型チタノシリケートの調製とフェノール酸化への応用2019

    • Author(s)
      石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第124回触媒討論会 討論会A予稿集
    • Related Report
      2019 Annual Research Report
  • [Presentation] 新規骨格チタノシリケートTi-YNU-5を触媒とする選択酸化反応2019

    • Author(s)
      淺沼 開,石塚 遼,稲垣怜史,窪田好浩
    • Organizer
      第124回触媒討論会 討論会A予稿集
    • Related Report
      2019 Annual Research Report
  • [Presentation] AFX型ゼオライトの骨格内Al分布の制御2019

    • Author(s)
      稲垣怜史,難波晃史,石塚 遼,窪田好浩
    • Organizer
      第124回触媒討論会 討論会A予稿集
    • Related Report
      2019 Annual Research Report
  • [Presentation] Al含有量の多いMSE型ゼオライトの二段階酸処理による骨格構造の安定化と脱Al2019

    • Author(s)
      難波晃史,韓 喬,稲垣怜史,窪田好浩
    • Organizer
      第124回触媒討論会 討論会A予稿集
    • Related Report
      2019 Annual Research Report
  • [Presentation] Control of Selectivity in the Phenol Oxidation with H2O2 over Multi-dimensional Large-pore Titanosilicates2019

    • Author(s)
      S. Inagaki, M. Takeyama, R. Ishiduka, K. Asanuma, Y. Kubota
    • Organizer
      EuropaCat 2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis investigation of *STO-type zeolite by using uunconventional structure-directing agent2019

    • Author(s)
      Q. Liu, N. Nakazawa, S. Inagaki, Y. Kubota
    • Organizer
      19th International Zeolite Conference
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis and framework stabilization of new zeolite YNU-5 toward catalytic application2019

    • Author(s)
      N. Nakazawa, Y. Yoshida, S. Inagaki, Y. Kubota
    • Organizer
      19th International Zeolite Conference
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 新規骨格ゼオライトYNU-5へのTi導入と選択酸化触媒反応への応用2019

    • Author(s)
      淺沼 開,武山芽生,石塚 遼,岩井美帆,稲垣怜史,窪田好浩
    • Organizer
      第8回JACI/GSCシンポジウム
    • Related Report
      2019 Annual Research Report
  • [Remarks] Kubota Lab

    • URL

      http://www.kubota.ynu.ac.jp/

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report 2019 Annual Research Report
  • [Patent(Industrial Property Rights)] チタノシリケートとその製造方法2019

    • Inventor(s)
      窪田好浩、稲垣怜史、中澤直人、吉田友香、淺沼 開
    • Industrial Property Rights Holder
      国立大学法人横浜国立大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2019-095397
    • Filing Date
      2019
    • Related Report
      2019 Annual Research Report

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

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