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Catalytic Performance of Active Species Prepared in Hydrophobic Mesoporous Materials

Research Project

Project/Area Number 16560675
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Catalyst/Resource chemical process
Research InstitutionTokyo Institute of Technology

Principal Investigator

BABA Toshihide  Tokyo Institute of Technology, Interdisciplinary Graduate School of Science and Engineering, Professor, 大学院・総合理工学研究科, 教授 (50165057)

Project Period (FY) 2004 – 2005
Project Status Completed (Fiscal Year 2005)
Budget Amount *help
¥3,200,000 (Direct Cost: ¥3,200,000)
Fiscal Year 2005: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2004: ¥2,500,000 (Direct Cost: ¥2,500,000)
Keywordsmethane / ethene / propene / Zeolite / silver cations / カルベニウムイオン / 銀イオンクラスター / メチル化反応 / ベンゼン / トルエン / メソポーラス物質 / 疎水性 / 有機ー無幾ハイブリッド / ブレンステッド酸 / ルイス酸 / スルホ基
Research Abstract

The heterolytic dissociation of methane over silver cationic clusters (Ag_n^+) in Ag^+-exchanged zeolites, leading to the formation of silver hydride (Ag_n-H) and CH_3^<δ+> species, which reacts with ethene to form propene around 673 K. Methane conversion of 13.2% is achieved at 673 K over Ag-ZSM-5 catalyst to form higher hydrocarbons, such as propene and toluene. Under these reaction conditions, H-ZSM-5 does not catalyze the methane conversion, only ethene being converted into higher hydrocarbons. The reaction of methane with benzene also proceeded to form toluene and xylenes over Ag-ZSM-5 at 673 K. Zeolites exchanged with metal cations such as In and Ga also activate methane in the presence of ethene. Using ^<13>C-labeled methane as a reactant, propene is shown to be a primary product from by methane and ethene. Thus, a significant proportion of propene was singly ^<13>C-labeled (^<13>CC_2H_6). When In-ZSM-5 was used as a catalyst, not only propene, but also benzene and toluene were formed. ^<13>C atoms were not found in benzene molecules produced, indicating that benzene is entirely originated from ethene. On the other hand, in toluene, ^<13>C atoms are found in toluene, and singly ^<13>C-labeled toluene (^<13>CC_6H_8) was formed. This implies that toluene is formed by the reaction of benzene with methane, though there is a possibility that it is formed by the reaction of propene with n-butenes formed by the dimerization of ethene. The former the reaction path was confirmed by direct reaction of ^<13> _CH_4 with benzene.

Report

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

    (13 results)

All 2006 2005 2004 Other

All Journal Article (13 results)

  • [Journal Article] Heterolytic Dissociation of C-H Bond of Methane over Ag^+-exchanged Zeolites and Conversion of Methane into Higher Hydrocarbons in the Presence of Ethene or Benzene2006

    • Author(s)
      Toshihide Baba, Koji Inazu
    • Journal Title

      Chem. Lett. 35

      Pages: 142-147

    • NAID

      10017166618

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Heterolytic Dissociation of C-H Bond of Methane over Ag^+-exchanged Zeolites and Conversion of Methane into Higher Hydrocarbons in the Presence of Ethene or Benzene2006

    • Author(s)
      Toshihide Baba, Koji Inazu
    • Journal Title

      Chem.Lett., High light review 35

      Pages: 142-147

    • NAID

      10017166618

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Selective Transesterification of Triorein with Methanol to Methyl Oleate and Glycerol with Alkali Metal Salts Loaded on Alumina as Solid Base Catalysts2005

    • Author(s)
      Takahiro Ebiura, Tsuneo Echizen, Akio Ishikawa, Kazuhito Murai, Toshihide Baba
    • Journal Title

      Appl. Catal. A General 283

      Pages: 111-116

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Catalytic Transformation of Methane over In-loaded ZSM-5 Zeolite in the Presence of Ethene2005

    • Author(s)
      Toshihide Baba, Yoshimune Abe, Kenji Nomoto, Ko-ji Inaz, Stuneo Echizen, Akio Ishikawai, Kazuhito Murai
    • Journal Title

      J. Phys. Chem. 109

      Pages: 4263-4268

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Conversion of Methane over Ag^+-exchanged Zeolite in the Presence of Ethene2005

    • Author(s)
      Toshihide Baba
    • Journal Title

      Catalysis Survey from Asia 9

      Pages: 147-154

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Selective Transesterification of Triorein with Methanol to Methyl Oleate and Glycerol with Alkali Metal Salts Loaded on Alumina as Solid Base Catalysts2005

    • Author(s)
      Takahiro Ebiura, Tsuneo Echizen, Akio Ishikawa, Kazuhito Murai, Toshihide Baba
    • Journal Title

      Appl.Catal.A General 283

      Pages: 111-116

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Catalytic Transformation of Methane over In-loaded ZSM-5 Zeolite in the Presence of Ethene2005

    • Author(s)
      Toshihide Baba, Yoshimune Abe, Kenji Nomoto, Ko-ji Inaz, Stuneo Echizen, Akio, Ishikawai, Kazuhito Murai
    • Journal Title

      J.Phys.Chem. 109

      Pages: 4263-4268

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Conversion of Methane over Ag^+-exchanged Zeolite in the Presence of Ethene2005

    • Author(s)
      Toshihide Baba
    • Journal Title

      Catalysis Survey from Asia 9(3)

      Pages: 147-154

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Catalytic Transformation of Methane over In-loaded ZSM-5 Zeolite in the Presence of Ethene2005

    • Author(s)
      Toshihide Baba, Yoshimune Abe, Kenji Nomoto, Ko-ji Inaz, Stuneo Echizen, Akio Ishikawai, Kazuhito Murai
    • Journal Title

      J.Phys.Chem.B 109

      Pages: 4263-4268

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Characterization of Ag^+-Exchanged Zeolite A with H_2 and CO Adsorption by FTIR2004

    • Author(s)
      Ping Wang, Shuwu Yang, Junko N.Kondo, Kazunari Domen, Toshihide Baba
    • Journal Title

      Bull. Chem. Soc. Jpn 77

      Pages: 1627-1634

    • NAID

      10013584217

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Asymmetric Micheal addition reaction of 2-sililyoxyfurans catalyzed by binaphthyldiimine-Ni(II) complexes2004

    • Author(s)
      H.Suga, T.Kitamura, T.Baba
    • Journal Title

      Chemical Communications

      Pages: 1414-1415

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Characterization of Ag^+-Exchanged Zeolite A with H_2 and CO Adsorption by FTIR2004

    • Author(s)
      P.Wang, S.Yang, J.N.Kondo, K.Domen, T.Baba
    • Journal Title

      Bulletin Chemical Society of Japan 77

      Pages: 1627-1634

    • NAID

      10013584217

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Characterization of Ag^+-Exchanged Zeolite A with H_2 and CO Adsorption by FTIR

    • Author(s)
      Ping Wang, Shuwu Yang, Junko N.Kondeo, Kazunari Domen, Toshihide Baba
    • Journal Title

      Bull.Chem.Soc.Jpn. 7

      Pages: 1627-1634

    • NAID

      10013584217

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary

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Published: 2004-04-01   Modified: 2016-04-21  

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