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Synthesis of novel microporous materials based on the elucidation of formation of zeolites in nanolevel

Research Project

Project/Area Number 15360426
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Catalyst/Resource chemical process
Research InstitutionThe University of Tokyo

Principal Investigator

OKUBO Tatsuya  The University of Tokyo, Graduate School of Engineering, Associate Professor, 大学院工学系研究科, 助教授 (40203731)

Co-Investigator(Kenkyū-buntansha) OGURA Masaru  The University of Tokyo, Graduate School of Engineering, Associate Professor, 生産技術研究所, 助教授 (50298155)
KOHARA Shinji  SPring-8, Researcher, 利用研究促進部門, 副主幹研究員 (90360833)
YOKOI Toshiyuki  The University of Tokyo, Graduate School of Engineering, Research Associate, 大学院工学系研究科, 助手 (00401125)
Project Period (FY) 2003 – 2005
Project Status Completed (Fiscal Year 2005)
Budget Amount *help
¥15,300,000 (Direct Cost: ¥15,300,000)
Fiscal Year 2005: ¥3,700,000 (Direct Cost: ¥3,700,000)
Fiscal Year 2004: ¥3,700,000 (Direct Cost: ¥3,700,000)
Fiscal Year 2003: ¥7,900,000 (Direct Cost: ¥7,900,000)
Keywordszeolite / nucleation / crystal growth / synchrotron radiation / high energy XRD / small angle X-ray scattering / in situ observation / precursor / 高エネルギーX線回折 / 前駆体 / in-situ測定
Research Abstract

In this research project, investigation on zeolite precursors during the stages of nucleation and crystal growth is performed at the level of atomic scale by means of various in situ characterization techniques. The formation process of zeolite crystals is recognized here as a kind of reaction network.
As for the clarification of zeolite precursors, generation of ring structures which are composed of hetero-atoms such as oxides of Si, Al, and/or other metals, and the roles of alkali metals in the generation were focused on. High-Energy X-Ray Diffraction (HEXRD) is utilized for the investigation of ring structures of aluminosilicate species involved in the formation process of zeolites. We could clarify by the tool the critical roles of hetero-atoms on the ring species and of alkali metals on the assembly of the rings. We could successfully lead the conclusion that introduction of Al into the ring structure decreased the proportional contribution of odd-numbered rings, and the addition of Zn enhanced the formation of three-membered ring. It is noted that the ring number distribution is already determined in the amorphous phase of reactant aluminosilicate hydrogel prior to crystallization to each zeolitic phase. In the successive stage, nucleation and growth, we concluded that three kinds of particles of primary and secondary units and crystal exist in the aqueous phase of solution, by our original contribution using Small Angle X-ray Scattering(SAXS)-Wide Angle X-ray Scattering(WAXS) in situ measurement. We finally proposed a whole schematic process of crystallization of zeolite through these explorations.
We also succeeded to obtain much smaller nano-crystal of zeolite than previously reported, owing to the knowledge obtained above. In this method, nano-crystals at higher concentration were achieved to crystallize without addition of organic additives, which are conventionally accepted as an indispensable reagent for such a type of nano-crystal.

Report

(4 results)
  • 2005 Annual Research Report   Final Research Report Summary
  • 2004 Annual Research Report
  • 2003 Annual Research Report
  • Research Products

    (20 results)

All 2006 2005 2004 2003 Other

All Journal Article (18 results) Publications (2 results)

  • [Journal Article] Phase Selection of FAU and LTA Zeolites by Controlling Synthesis Parameters2006

    • Author(s)
      Toru Wakihara, Shinji Kohara, Gopinathane Sankar, Seijiro Saito, Manuel Sanchez-Sanchez, Adrian R.Overweg, Wei Fan, Masaru Ogura, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 8

      Pages: 224-227

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Phase Selection of FAU and LTA Zeolites by Controlling Synthesis Parameters2006

    • Author(s)
      Wei Fan, Satoshi Shirato, Gao Feifei, Masaru Ogura, Tatsuya Okubo
    • Journal Title

      Microporous and Mesoporous Materials 89

      Pages: 227-234

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Annual Research Report 2005 Final Research Report Summary
  • [Journal Article] In Situ Observation of Homogeneous Nucleation of Nanosized Zeolite A2006

    • Author(s)
      Wei Fan, Matthew O'Brien, Masaru Ogura, Manuel Sanchez-Sanchez, Christopher Martin, Florian Meneau, Ken-ichi Kurumada, Gopinathan Sankar, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 8

      Pages: 1335-1339

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Annual Research Report 2005 Final Research Report Summary
  • [Journal Article] Atomic Architecture of Amorphous Zeolite Precursor Species2006

    • Author(s)
      Toni Wakihara, Shinji Kohara, Gopinathane Sankar, Seijiro Saito, Manuel Sanchez-Sanchez, Adrian R. Overweg, Wei Fan, Masaru Ogura, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 8

      Pages: 224-227

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Manuel Sanchez-Sanchez, Christopher Martin, Florian Meneau, Ken-ichi Kurumada, Gopinathan Sankar and Tatsuya Okubo, In Situ Observation of Homogeneous Nucleation of Nanosized Zeolite A2006

    • Author(s)
      Wei Fan, Matthew O'Brien, Masaru Ogura
    • Journal Title

      Physical Chemistry Chemical Physics 8

      Pages: 1335-1339

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Atomic Architecture of Amorphous Zeolite Precursor Species2006

    • Author(s)
      Toru Wakihara, Shinji Kohara, Gopinathane Sankar, Seijiro Saito, Manuel Sanchez-Sanchez, Adrian R.Overweg, Wei Fan, Masaru Ogura, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 8

      Pages: 224-227

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Investigation of the Surface Structure of Zeolite A2005

    • Author(s)
      Toru Wakihara, Yukichi Sasaki, Hitoshi Kato, Yuichi Ikuhara, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 7

      Pages: 3416-3418

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Annual Research Report 2005 Final Research Report Summary
  • [Journal Article] Investigation of the Surface Structure of Zeolite A2005

    • Author(s)
      Tom Wakihara, Yukichi Sasaki, Hitoshi Kato, Yuichi Ikuhara, Tatsuya Okubo
    • Journal Title

      Physical Chemistry Chemical Physics 7

      Pages: 3416-3418

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Crystal Growth Behavior of Zeolites Elucidated by Atomic Force Microscopy2004

    • Author(s)
      Toru Wakihara, Tatsuya Okubo
    • Journal Title

      Journal of Chemical Engineering of Japan 37

      Pages: 669-674

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Crystal Growth of Faujasite Observed by Atomic Force Microscopy, Microporous and Mesoporous Materials2004

    • Author(s)
      Toru Wakihara, Akira Sugiyama, Tatsuya Okubo
    • Journal Title

      Microporous and Mesoporous Materials 70

      Pages: 7-13

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary 2004 Annual Research Report
  • [Journal Article] Crystal Growth Behavior of Zeolites Elucidated by Atomic Force Microscopy2004

    • Author(s)
      Toni Wakihara, Tatsuya Okubo
    • Journal Title

      Journal of Chemical Engineering of Japan 37

      Pages: 669-674

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Crystal Growth of Faujasite Observed by Atomic Force Microscopy2004

    • Author(s)
      Toni Wakihara, Akira Sugiyama, Tatsuya Okubo
    • Journal Title

      Microporous and Mesoporous Materials 70

      Pages: 7-13

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Aluminosilicate Species in the Hydrogel Phase Formed during the Aging Process for the Crystallization of FAU Zeolite2003

    • Author(s)
      Masaru Ogura, Yasuyuki Kawazu, Hiroshi Takahashi, Tatsuya Okubo
    • Journal Title

      Chemistry of Materials 15・13

      Pages: 2661-2667

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Aluminosilicate Species in the Hydrogel Phase Formed during the Aging Process for the Crystallization of FAU Zeolite2003

    • Author(s)
      Masaru Ogura, Yasuyuki Kawazu, Hiroshi Takahashi, Tatsuya Okubo
    • Journal Title

      Chemistry of Materials 15

      Pages: 2661-2667

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] In situ small angle and wide angle X-ray scattering investigation on nucleation and crystal growth of nanosized zeolite A

    • Author(s)
      Wei Fan, Masaru Ogura, Gopinathan Sankar, Tatsuya Okubo
    • Journal Title

      Chemistry of Materials 印刷中

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] ROLE OF HETEROATOMS IN PRECURSOR FORMATION OF ZEOLITES

    • Author(s)
      Toru Wakihara, Wei Fan, Yasuhiro Suzuki, Masaru Ogura, Shinji Kohara, Gopinathan Sankar, Tatsuya Okubo
    • Journal Title

      Studies in Surface Science and Catalysis 印刷中

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] In situ small angle and wide angle X- ray scattering investigation on nucleation and crystal growth of nanosized zeolite A

    • Author(s)
      Wei Fan, Masaru Ogura, Gopinathan Sankar, Tatsuya Okubo
    • Journal Title

      Chem.Mater. (in press)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] ROLE OF HETEROATOMS IN PRECURSOR FORMATION OF ZEOLITES

    • Author(s)
      Toru Wakihara, Wei Fan, Yasuhiro Suzuki, Masaru Ogura, Shinji Kohara, Gopinathan Sankar, Tatsuya Okubo
    • Journal Title

      Stud.Surf.Sci.Catal. (in press)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Publications] Masaru Ogura, Yasuyuki Kawazu, Hiroshi Takahashi, Tatsuya Okubo: "Aluminosilicate Species in the Hydrogel Phase Formed during the Aging Process for the Crystallization of FAU Zeolite"Chemistry of Materials. 15・13. 2661-2667 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Toru Wakihara, Tatsuya Okubo: "Crystal Growth Behavior of Zeolites Elucidated by Atomic Force Microscopy"Journal of Chemical Engineering of Japan. (印刷中). (2004)

    • Related Report
      2003 Annual Research Report

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Published: 2003-04-01   Modified: 2016-04-21  

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