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Preparation of catalytic membranes with controlled structure and its application to membrane reaction

Research Project

Project/Area Number 13555216
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section展開研究
Research Field 反応・分離工学
Research InstitutionHIROSHIMA UNIVERSITY

Principal Investigator

TSURU Toshinori  Hiroshima University, Graduate School of Engineering, associate Professor, 大学院・工学研究科, 助教授 (20201642)

Co-Investigator(Kenkyū-buntansha) MUTOU Haruhiko  Fluent Asia Pacific Co., Ltd., Senior engineering, シニアエンジニア(研究職)
YOSHIOKA Tomohisa  Hiroshima University, Graduate School of Engineering, Research associate, 大学院・工学研究科, 助手 (50284162)
ASAEDA Masashi  Hiroshima University, Graduate school of Engineering, Professor, 大学院・工学研究科, 教授 (40026224)
YOSHIDA Kazuhiro  The Chugoku Power Co., Inc., Researcher, 技術研究所, 研究員(研究職)
Project Period (FY) 2001 – 2003
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥12,100,000 (Direct Cost: ¥12,100,000)
Fiscal Year 2003: ¥2,400,000 (Direct Cost: ¥2,400,000)
Fiscal Year 2002: ¥2,300,000 (Direct Cost: ¥2,300,000)
Fiscal Year 2001: ¥7,400,000 (Direct Cost: ¥7,400,000)
Keywordsmembrane reactor / catalytic membrane / zeolite membranes / silica membrane / methylation of toluene / steam reforming of methane / トルエン / メタノール / キシレン / メタン / 水蒸気改質 / ZSM膜
Research Abstract

Catalytic membrane reactors were investigated using two types of catalytic membranes : MFI membranes which had separation ability and catalytic activity in the top layer and silica membranes which had separation ability in the top layer and catalytic activity in the supporting layer.
MFI zeolite membranes having different Si/Al ratios were prepared by secondary growth of crystalline colloidal seeds under hydrothermal conditions. An MFI membrane of Si/Al=∞ showed a n-C_4H_<10> permeance of 1.5x10^<-5> m^3(STP)m^<-2>s^<-1>kPa^<-1> and a n/i-C_4H_<10> selectivity of 15 at 150℃. By addition of Al into MFI membranes, the zeolite layers appear to be randomly-oriented and n/i-C_4H_<10> selectivities were decreased. Methylation of toluene using MFI catalytic membrane reactors was carried out from 400-500 ℃. Toluene conversions increased with reaction temperature and p-xylene selectivity achieved was 80 % at maximal, suggesting the effectiveness of MFI catalytic membrane reactors.
Methane steam r … More eforming with and without added oxygen was theoretically and experimentally investigated using microporous silica membranes, which allow the permeation of hydrogen as well as other gases in reactants and products. A simulation of catalytic membrane reactors was carried out for a co-current, isothermal, and plug-flow-type membrane reactor with the selective permeation of hydrogen through microporous membranes. Catalytic membrane reactors, consisting of a silica microporous layer and a Ni-catalyst layer, were prepared. Catalytic membrane reactors showing a hydrogen selectivity over nitrogen of 30-100 with hydrogen permeances of 0.5-3x10^<-7> mol m^<-2>s^<-1>Pa^<-1> were applied to the steam reforming of methane with and without the addition of oxygen. The reaction was carried out at 500 ℃, and the feed and permeate pressure were maintained at 100 and 20 kPa, respectively. Methane conversion, X_<CH4>, increased up to approximately 0.8 beyond the equilibrium conversion of 0.44 by extracting hydrogen in permeate stream. Less

Report

(4 results)
  • 2003 Annual Research Report   Final Research Report Summary
  • 2002 Annual Research Report
  • 2001 Annual Research Report
  • Research Products

    (18 results)

All Other

All Publications (18 results)

  • [Publications] 都留稔了: "多孔質水素分離膜を用いたメタン改質の膜型反応シミュレーション"化学工学論文集. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Methane Steam Reforming by Catalytic Membrane Reactors Using Hydrogen-Permselective Microporous Silica Membranes and the Effect of Added"AIChE J.. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Catalytic membrane reactors for methane reforming using hydrogen permselective silica membranes"Transactions of Materials Research Society of Japan. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] 高田裕子: "Si/Al比の異なるMFI型ゼオライト薄膜の気体透過特性とトルエンのメチル化反応"化学工学論文集. 29. 427-431 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Characterization of sol-gel derived membranes and zeolite membranes nanopermporometry"Separation and Purification Technology. 32. 23-27 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "ZEOLITES : SEPARATION SCIENCE"Encyclopedia Supramolecular Chemistry. 24 (2004)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Simulation of Catalytic Membrane Reaction for Methane Reforming Using a Microporous Hydrogen Separation Membrane"Kagaku Kogaku Ronbunshu. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Methane Steam Reforming by Microporous Catalytic Membrane Reactor and Effect of Added Oxygen"AIChE J.. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] T.Tsuru: "Catalytic membrane reactors for methane reforming using hydrogen permselective silica membranes"Transactions of Materials Research Society of Japan. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Yuko Takata: "Gas Permeation Properties and Methylation of Toluene by MFI Zeolite Membranes with Different Si/Al Ratios"Kagaku Kogaku Ronbunshu. 29. 427-431 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "Characterization of sol-gel derived membranes and zeolite membranes nanopermporometry"Separation and Purification Technology. 32. 23-27 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] Toshinori Tsuru: "ZEOLITES : SEPARATION SCIENCE"Encyclopedia Supramolecular Chemistry.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] 都留稔了: "多孔質水素分離膜を用いたメタン改質の膜型反応シミュレーション"化学工学論文集. accepted. (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] Toshinori Tsuru: "Methane Steam Reforming by Catalytic Membrane Reactors Using Hydrogen-Permselective Microporous Silica Membranes and the Effect of Added Oxygen"AIChE J.. accepted. (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] Toshinori Tsuru: "Catalytic membrane reactors for methane reforming using hydrogen permselectiv e silica membranes"Transactions of Materials Research Society of Japan. accepted. (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] 高田裕子: "Si/Al比の異なるMFI型ゼオライト薄膜の気体透過特性とトルエンのメチル化反応"科学工学論文集. (accepted). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Toshinori Tsuru: "ZEOLITES : SEPARATION SCIENCE"Encyclopedia Supramolecular Chemistry. (accepted). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] Yuko Takata: "Gas permeation properties of MFI zeolite membranes prepared by the secondary growth of colloidal silicalite and application to the methylation of"Microporous and Mesoporous Materials. 54. 257-268 (2002)

    • Related Report
      2002 Annual Research Report

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Published: 2001-04-01   Modified: 2016-04-21  

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