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Development of a novel catalyst for direct conversion of low valued natural gas containing carbon dioxide to petrochemical feedstock

Research Project

Project/Area Number 14350422
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionTohoku University

Principal Investigator

OHTSUKA Yasuo  Tohoku University, Institute of Multidisciplinary Research for Advanced Materials, Professor, 多元物質科学研究所, 教授 (20091663)

Co-Investigator(Kenkyū-buntansha) TSUBOUCHI Naoto  Tohoku University, Institute of Multidisciplinary Research for Advanced Materials, Research Associate, 多元物質科学研究所, 助手 (90333898)
KIKUCHI Takemitsu  Tohoku University, Institute of Multidisciplinary Research for Advanced Materials, Research Associate, 多元物質科学研究所, 助手 (30169825)
Project Period (FY) 2002 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥16,000,000 (Direct Cost: ¥16,000,000)
Fiscal Year 2004: ¥3,400,000 (Direct Cost: ¥3,400,000)
Fiscal Year 2003: ¥6,000,000 (Direct Cost: ¥6,000,000)
Fiscal Year 2002: ¥6,600,000 (Direct Cost: ¥6,600,000)
KeywordsNatural gas / Carbon dioxide / Petrochemical feedstock / Binary oxide catalysts / Silica supports / 酸化物触媒 / メソポーラスシリカ
Research Abstract

The present work focuses on developing a novel catalyst system for the purpose of directly converting low valued natural gas, which contains a large amount of CO_2, into petrochemical feedstock such as ethane and ethylene, in other words, for CH_4 coupling with CO_2 to produce C_2 hydrocarbons. In an unsupported binary oxide catalyst, which is composed of Mn oxide and alkaline earth metal oxide, C_2 selectivity increases in the order of Ca-Mn < Ba-Mn < Sr-Mn, and the value over the Sr-Mn catalyst reaches 80%, which is higher than those over Ca-Ce and Ca-Cr catalysts. The Ba-Mn and Sr-Mn provide almost no dependency of C_2 selectivity on partial pressure of CO_2 in feed gas, in contrast with the remarkable dependency observed with Ca based composite oxides. It is likely that this difference originates from chemical structures of catalytically active species and the mechanism of C_2 formation. When these oxide components are impregnated with a mesoporous molecular sieve silica (SBA-15) with high surface area (880m^2/g) and large pore volume (1.9cm^3/g), almost all of the oxide species can be held inside the mesopores with average pore diameter of 7.4nm, and C_2 selectivity is larger with Mn-based composites, whereas space time yield of C_2 hydrocarbons is higher with Ca-based composites. The use of conventional amorphous SiO_2 supports in place of the SBA-15 support shows that, although C_2 selectivity is larger with the latter, the yield of C_2 hydrocarbons is the highest with the Ca-Ce catalyst supported on the SiO_2 with the lowest surface area of 300m^2/g. To improve the selectivity over the supported Ca-Ce catalyst maybe the subject of future study.

Report

(4 results)
  • 2004 Annual Research Report   Final Research Report Summary
  • 2003 Annual Research Report
  • 2002 Annual Research Report
  • Research Products

    (14 results)

All 2005 2004 2003 2002 Other

All Journal Article (9 results) Book (2 results) Publications (3 results)

  • [Journal Article] Formation of C_2 hydrocarbons by the reaction of methane and carbon dioxide with supported metal oxide catalysts2005

    • Author(s)
      Y.Ohtsuka
    • Journal Title

      Amer.Chem.Soc.Div.Fuel Chem. 50・2(発表予定)

    • Related Report
      2004 Annual Research Report
  • [Journal Article] シリカ担持触媒を用いるメタンと二酸化炭素の反応2004

    • Author(s)
      菊地 毅光
    • Journal Title

      平成16年度化学系9学協会連合東北地方大会講演予稿集

      Pages: 101-101

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Catalysis of the reaction of methane and carbon dioxide with silica-supported catalysts2004

    • Author(s)
      T.Kikuchi
    • Journal Title

      The 2004 Tohoku Region Fall Meeting of the Chemical Society of Japan

      Pages: 101-101

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] シリカ担持触媒を用いるメタンと二酸化炭素の反応2004

    • Author(s)
      菊地毅光
    • Journal Title

      平成16年度化学系学協会東北大会講演予稿集

      Pages: 101-101

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Catalysis of methane coupling with carbon dioxide over binary oxides2003

    • Author(s)
      Y.Wang
    • Journal Title

      Topics in Catalysis 22

      Pages: 71-75

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] メソポーラスシリカ担持触媒を用いるメタンと二酸化炭素の反応2003

    • Author(s)
      菊地 毅光
    • Journal Title

      平成15年度化学系9学協会連合東北地方大会講演予稿集

      Pages: 113-113

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Catalytic performances of binary metal oxides in methane coupling with carbon dioxide2003

    • Author(s)
      Y.Wang
    • Journal Title

      Proceedings of The 8^<th> Japan-China Symposium on Coal and C_1 Chemistry

      Pages: 143-144

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Conversion of methane with carbon dioxide over several catalysts supported on mesoporous molecular-sieving silica2003

    • Author(s)
      T.Kikuchi
    • Journal Title

      The 2003 Tohoku Region Fall Meeting of the Chemical Society of Japan

      Pages: 113-113

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Catalytic performances of binary metal oxides in methane coupling with carbon dioxide2003

    • Author(s)
      Y.Wang
    • Journal Title

      Proc.,The 8^<th> Japan-China Symposium on Coal and C_1 Chemistry

      Pages: 143-144

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Book] Utilization of carbon dioxide for direct, selective conversion of methane to ethane and ethylene with calcium-based binary catalysts2002

    • Author(s)
      Ye Wang
    • Total Pages
      17
    • Publisher
      American Chemical Society
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Book] Utilization of carbon dioxide for direct, selective conversion of methane to ethane and ethylene with calcium-based binary catalysts2002

    • Author(s)
      Y.Wang
    • Publisher
      American Chemical Society
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Publications] Y.Wang, T.Kikuchi, N.Tsubouchi, Y.Ohtsuka: "Catalytic performances of binary metal oxides in methane coupling with carbon dioxide"The 8^<th> Japan-China Symposium on Coal and C_1 Chemistry. 143-144 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 菊地毅光, 坪内直人, 大塚康夫: "メソポーラスシリカ担持触媒を用いるメタンと二酸化炭素の反応"平成15年度化学系9学協会連合東北地方大会講演予稿集. 113 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Ohtsuka: "Catalytic performances of binary metal oxides in methane coupling with carbon dioxide"The 8^<th> Japan-China Symposium on Coal and C1 Chemistry. (To be presented). (2003)

    • Related Report
      2002 Annual Research Report

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Published: 2002-04-01   Modified: 2016-04-21  

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