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Design for a shape-selective oxidation reaction system using zeolite nanocrystal-layered membrane

Research Project

Project/Area Number 17360379
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Reaction engineering/Process system
Research InstitutionHOKKAIDO UNIVERSITY

Principal Investigator

MASUDA Taka  Hokkaido Univ., Grad. School of Eng., Professor, 大学院工学研究科, 教授 (20165715)

Co-Investigator(Kenkyū-buntansha) TAGO Teruoki  Hokkaido Univ., Grad. School of Eng., Associate Professor, 大学院工学研究科, 助教授 (20304743)
辻 俊郎  北海道大学, 大学院・工学研究科, 助教授 (30163794)
Project Period (FY) 2005 – 2006
Project Status Completed (Fiscal Year 2006)
Budget Amount *help
¥15,700,000 (Direct Cost: ¥15,700,000)
Fiscal Year 2006: ¥6,600,000 (Direct Cost: ¥6,600,000)
Fiscal Year 2005: ¥9,100,000 (Direct Cost: ¥9,100,000)
Keywordszeolite / nanocrystal / selective oxidation / selective deactivation of acid site / Ni-supporting zeolite / nanocrystal-layered membrane / catalytic membrane / Ni固定化ゼオライト / 拡散 / マイクロエマルション / 部分酸化 / 逐次反応 / 透過速度
Research Abstract

The main objective of this research is to develop a zeolite membrane exhibiting shape-selective oxidation properties. The major results are described below.
A)Preparation of mono-dispersed ZSM-5 zeolite nanocrystals: Two types of zeolites with different crystal size, 2.0 micro-meter (micro-zeolite) and 50 nano-meter (nano-zeolite), could be prepared. These zeolites show the same acidity, pore volume, and crystalinity regardless of the different crystal size. Methanol reaction was carried out over the ZSM-5 zeolites, which is a series of reactions from methanol to ether, olefins, paraffins, and aromatics. Though the decrease in the catalytic activity was observed just after the reaction in the micro-zeolite, the nano-zeolite exhibited the high activity and the long life-time.
B)Selective-deactivation of the acid sites at the outer surface: Acid sites of the zeolite at the outer surface were successfully deactivated by using phenyl-slilane compound. The intermediate of the dimthyl-ether could be selectively produced over the zeolite.
C)Preparation of nanocrystal-layered membrane: The ZSM-5 zeolite nanocrystals were piled up on an alumina filter. The thickness of the nanocrystals could be controlled in the range from 20 to 40 micrometer. The methanol reaction was carried out using the nanocrystal-layered membrane, and the selectivity of the intermediate such as ether and olefins successfully increased up to 90 %.
D)Ni-supporting zeolite for selective-oxidation system: Since the acid sites at the outer surface of the zeolite were deactivated, Ni ions could be selectively exchanged for protons at the inner pore of the ZSM-5 zeolite nanocrystals. Accordingly, Ni-supporting zeolite nanocrystals and membrane, which realizes the shape-selective oxidation, could be prepared.

Report

(3 results)
  • 2006 Annual Research Report   Final Research Report Summary
  • 2005 Annual Research Report
  • Research Products

    (21 results)

All 2007 2006 2005 Other

All Journal Article (19 results) Patent(Industrial Property Rights) (2 results)

  • [Journal Article] Preparation of hydrophilic silicalite-1 nanocrystal-layered membrane for separation of water from water-acetone solution by pervaporation2007

    • Author(s)
      T.Tago et al.
    • Journal Title

      Studies in Surface Science and Catalysis (In press)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Network structure consisting of chain-like arrays of gold nanoparticles and silica layer prepared using a nonionic reverse-micelle template2006

    • Author(s)
      H.Mastune et al.
    • Journal Title

      Journal of Nanoparticle Research 8

      Pages: 1083-1087

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Preparation of Monolithic SiO2-Al2O3 Cryogels with Inter-Connected Macropores through Ice-Templating2006

    • Author(s)
      H.Nishihara et al.
    • Journal Title

      Journal of Materials Chemistry 16

      Pages: 3231-3236

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Preparation of Mono-Dispersed MFI-type Zeolite Nanocrystals via Hydrothermal Synthesis in Water/Surfactant/Oil Solution2006

    • Author(s)
      T.Tago et al.
    • Journal Title

      Studies in Surface Science and Catalysis 159

      Pages: 185-188

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Network structure consisting of chain-like arrays of gold nanoparticles and silica layer prepared using a nonionic reverse-micelle template2006

    • Author(s)
      H.Matsune, T.Tago, K.Shibata, K.Wakabayashi, M.Kishida
    • Journal Title

      Journal of Nanoparticle Research 8

      Pages: 1083-1087

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Preparation of Monolithic SiO2-A12O3 Cryogels with Inter Connected Macropores through Ice-Templating2006

    • Author(s)
      H.Nishihara, S.R.Mukai, Y.Fujii, T.Tago, T.Masuda, H.Tamon
    • Journal Title

      Journal of Materials Chemistry 16

      Pages: 3231-3236

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Preparation of Mono-Dispersed MFI-type Zeolite Nanocrystals via Hydrothermal Synthesis in Water/Surfactant/Oil Solution2006

    • Author(s)
      T.Tago, K.Iwakai, M.Nishi, T.Masuda
    • Journal Title

      Studies in Surface Science and Catalysis 159

      Pages: 185-188

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Preparation of Mono-Dispersed MFI-type Zeolite Nanocrystals via Hydrothermal Synthesis in Water/Surfactant/Oil Solution2006

    • Author(s)
      T.Tago
    • Journal Title

      Studies in Surface Science and Catalysis 159

      Pages: 185-188

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Recovery of Lighter Fuels from Petroleum Residual Oil by Oxidative Cracking with Steam over Zr-Al-FeOx2006

    • Author(s)
      E.Fumoto
    • Journal Title

      Chemistry Letters 35(9)

      Pages: 998-999

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Preparation of Monolithic Si02-A1203 Cryogels with Inter-Connected Macropores through Ice-Templating2006

    • Author(s)
      H.Nishihara
    • Journal Title

      Journal of Materials Chemistry 16

      Pages: 3231-3236

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Production of Ketones from sewage sludge over zirconia-supporting iron oxide catalysts in steam atmosphere2006

    • Author(s)
      E.Fumoto
    • Journal Title

      Applied Catalysis B, Enviromental 68

      Pages: 154-159

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Production of Lighter Fuels by Cracking Petroleum Residual Oil with Steam over Zirconia-Supporting Iron Oxide Catalysts2006

    • Author(s)
      E.Fumoto
    • Journal Title

      Energy and Fuels 20(1)

      Pages: 1-6

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Simultaneous Characterization of Acidic and Basic Properties of Solid Catalysts by a New TPD Method and Their Correlation to Reaction Rates2005

    • Author(s)
      T.Tago et al.
    • Journal Title

      Applied Catalysis, A : General 290

      Pages: 54-64

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Control of Acid-site Location of ZSM-5 Zeolite Membrane and Its Application to the MTO Reaction2005

    • Author(s)
      T.Tago et al.
    • Journal Title

      Catalysis Today 105

      Pages: 662-666

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Simultaneous Characterization of Acidic and Basic Properties of Solid Catalysts by a New TPD Method and Their Correlation to Reaction Rates2005

    • Author(s)
      T.Tago, Y.Okubo, S.R.Mukai, T Tanaka, T.Masuda
    • Journal Title

      Applied Catalysis, A : General 290

      Pages: 54-64

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Control of Acid-site Location of ZSM-5 Zeolite Membrane and Its Application to the MTO Reaction2005

    • Author(s)
      T.Tago, K.Iwakai, K.Morita, K.Tanaka, T Masuda
    • Journal Title

      Catalysis Today 105

      Pages: 662-666

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Journal Article] Control of Acid-site Location of ZSM-5 Zeolite Membrane and Its Application to the MTO Reaction2005

    • Author(s)
      T.Tago, K.Iwakai, K.Morita, K.Tanaka, T.Masuda
    • Journal Title

      Catalysis Today 105

      Pages: 662-666

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Simultaneous Characterization of Acidic and Basic Properties of Solid Catalysts by a New TPD Method and Their Correlation to Reaction Rates2005

    • Author(s)
      T.Tago, Y.Okubo, S.R.Mukai, T.Tanaka, T.Masuda
    • Journal Title

      Applied Catalysis, A : General 290

      Pages: 54-64

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Preparation of hydrophilic silicalite-1 nanocrystal-layered membrane for separation of water from water-acetone solution by pervaporation

    • Author(s)
      T.Tago, Y.Nakasaka, A.Kayouda, T.Masuda
    • Journal Title

      Separation & Purification Technology (in press)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2006 Final Research Report Summary
  • [Patent(Industrial Property Rights)] 無機分離膜及びその製造方法2005

    • Inventor(s)
      増田隆夫, 多湖輝興
    • Industrial Property Rights Holder
      北海道大学, 日本碍子
    • Industrial Property Number
      2005-153451
    • Filing Date
      2005-05-26
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2006 Annual Research Report 2006 Final Research Report Summary
  • [Patent(Industrial Property Rights)] 無機分離膜及びその製造方法2005

    • Inventor(s)
      増田 隆夫, 多湖 輝興, 吉田 修一, 冨田 俊弘, 鈴木 憲次
    • Industrial Property Rights Holder
      日本ガイシ(株), 国立大学法人北海道大学
    • Industrial Property Number
      2005-153451
    • Filing Date
      2005-05-26
    • Related Report
      2005 Annual Research Report

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Published: 2005-04-01   Modified: 2016-04-21  

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