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Development of Aluminum-Gallium Mixed Oxide Catalysts for Selective Catalytic Reduction of NOx with methane

Research Project

Project/Area Number 15310053
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Environmental technology/Environmental materials
Research InstitutionKyoto University

Principal Investigator

INOUE Masashi  Kyoto University, Graduate School of Engineering, Professor (30151624)

Co-Investigator(Kenkyū-buntansha) IWAMOTO Shiniji  Kyoto University, Graduate School of Engineering, Research Associate (50252482)
Project Period (FY) 2003 – 2005
Project Status Completed (Fiscal Year 2005)
Budget Amount *help
¥15,700,000 (Direct Cost: ¥15,700,000)
Fiscal Year 2005: ¥4,000,000 (Direct Cost: ¥4,000,000)
Fiscal Year 2004: ¥2,900,000 (Direct Cost: ¥2,900,000)
Fiscal Year 2003: ¥8,800,000 (Direct Cost: ¥8,800,000)
KeywordsDeNOx reaction / Methane-SCR / Glycothermal reaction / Solvothermal reaction / Defect spinel / Catalyst / Nitrogen oxides / Gallia / ソルボサーマル反応 / γ-アルミナ / ガンマ型酸化ガリウム / 固溶体 / 複合酸化物触媒 / メタン脱硝 / グリコサーマル反応 / ガリウム / 結晶性 / NO選択還元反応 / 天然ガス / スピネル型複合酸化物 / 酸化物触媒 / 排煙脱硝
Research Abstract

Glycothermal synthesis of Ga2O3-Al2O3 solid solution was explored and it was found that the reaction of mixtures of aluminum isoproxide and gallium acetylacetonate in 1,4-butanediol or 1,5-pentanediol at 300℃ for 2 h yielded gamma-type Ga2O3-Al2O3 mixed oxides having a defect spinel structure, in which gallium ions selectively occupy the tetrahedral sites while aluminum ions preferentially occupy the octahedral sites. The Ga2O3-Al2O3 catalyst prepared by the glycothermal method had higher activity than those prepared by the corprecipitation or sol-gel method for selective catalytic reduction of Nox with methane. The activity of the catalyst prepared by the glycothermal method correlated with the ratio of the tetrahedral Ga ions to the total Ga ions and therefore it was concluded that the tetrahedral Ga ions with Al ions at the next-nearest-neighbor sites is the active site for the reaction. B-or Zn-modified solid solutions prepared by the addition of trimethyl borate or zinc acetate to … More the above-mentioned glycothermal reaction also had high activities for the deNOx reaction with methane. For the Zn-modified Ga2O3-Al2O3 catalyst, the modification rather reduced the population of the tetrahedral Ga sites but increased the crystallinity of the catalyst, which reduced the amount of adsorbed water, thus reducing the inhibitory effect of water caused by competitive adsorption of water with Nox or methane. In the selective catalytic reduction of Nox with methane, activation of methane is the rate-determining step and water is strongly adsorbed on the catalysts, thus inhibiting the catalytic activity. Therefore, the catalyst with high crystallinity had high activity. The solvothermal synthesis of the Ga2O3-Al2O3 mixed oxide in various solvents was examined and it was found that the reaction in diethylenetriamine gave the mixed oxide with high crystallinity. The catalyst prepared in diethylenetriamine had a quite high activity for selective catalytic reduction of Nox with methane. Less

Report

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

    (20 results)

All 2007 2006 2005 2004 Other

All Journal Article (15 results) (of which Peer Reviewed: 3 results) Presentation (2 results) Book (2 results) Publications (1 results)

  • [Journal Article] Performance of Solvothermally Prepared Ga_2O_3-Al_2O_3 Catalysts for SCR of NO with Methane2007

    • Author(s)
      M. Takahashi, T. Nakatani, S. Iwamoto, M. Inoue, et. al.
    • Journal Title

      Appi. Catal. B : Environmental 70

      Pages: 73-79

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Glycothermal Synthesis of γ-Ga_20_3-Al_2O_3 Solid Solutions2006

    • Author(s)
      M.Takahashi, N.Inoue, S.Iwamoto, M.Inoue, 他2名
    • Journal Title

      J.Am.Ceram.Soc. 87

      Pages: 2158-2166

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Selective Catalytic Reduction of NO with Methane on γ-Ga_2O_3-Al_2O_3 Solid Solutions Prepared by the Glycothermal Method2006

    • Author(s)
      M.Takahashi, N.Inoue, S.Iwamoto, M.Inoue, 他3名
    • Journal Title

      Appl.Catal.B:Environmental 65

      Pages: 142-149

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Effect of the Composition of Spinel Type Ga_2O_3-Al_2O_3-ZnO Catalysts on Activity for CH_4-SCR of NO and Optimization of Catalyst Composition2006

    • Author(s)
      M.Takahashi, T.Nakatani, S.Iwamoto, M.Inoue, 他2名
    • Journal Title

      Ind.Eng.Chem.Res. 45

      Pages: 3678-3683

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
    • Peer Reviewed
  • [Journal Article] Glycothermal Synthesis of γGa_2O_3-Al_2O_3 Solid Solutions2006

    • Author(s)
      M. Takahashi, N. Inoue, S. Iwamoto, M. Inoue, et. al.
    • Journal Title

      J. Am. Ceram. Soc, 87

      Pages: 2158-2166

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Selective Catalytic Reduction of NO with Methane on γ-Ga_2O_3-Al_2O_3 Solid Solutions Prepared by the Glycothermal Method2006

    • Author(s)
      M. Takahashi, N. Inoue, S., Iwamoto, M. Inoue, et. al.
    • Journal Title

      Appi. Catal. B : Environmental 65

      Pages: 142-149

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Effect of the Composition of Spinel Type Ga_20_3-Al_2O_3-ZnO Catalysts on Activity for CH_4-SCR of NO and Optimization of Catalyst Composition2006

    • Author(s)
      M. Takahashi, T. Nakatani, S. Iwamoto, M. Inoue, et. al.
    • Journal Title

      md. Eng. Chem. Res. 45

      Pages: 3678-3686

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Effect of Modification of Alkali on the γ-Ga_2O_3-Al_2O_3 Catalysts for SCR of NO with Methane2006

    • Author(s)
      M. Takahashi, T. Nakatani, S. Iwamoto, M. Inoue, et. al.
    • Journal Title

      J. Phys. Condensed Matter 18

      Pages: 5745-5757

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Solvothermal Synthesis2005

    • Author(s)
      M. Inoue
    • Journal Title

      Chemical Processing of Ceramics 2nd Ed. ; ed. by B. Lee and S.Komarneni Tayler & Trancis, Boca Raton, chapter 2

      Pages: 21-63

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Performance of Solvothermally Prepared Ga_2O_3-Al_2O_3 Catalysts for SCR of NO with Methane

    • Author(s)
      M.Takahashi, T.Nakatani, S.Iwamoto, T.Watanabe, M.Inoue
    • Journal Title

      Applied Catalysis B : Environmental (印刷中)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Selective Catalytic Reduction of NO with Methane on γ-Ga_2O_3-Al_2O_3 Solid Solutions Prepared by the Glycothermal Method

    • Author(s)
      M.Takahashi, N.Inoue, T.Nakatani, T.Takeguchi, S.Iwamoto, T.Watanabe, M.Inoue
    • Journal Title

      Applied Catalysis B : Environmental (印刷中)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Effect of the Composition of Spinel-Type Ga_2O_3-Al_2O_3-ZnO Catalysts on Activity for the CH_4-SCR of NO and Optimization of Catalyst Composition

    • Author(s)
      M.Takahashi, T.Nakatani, S.Iwamoto, T.Watanabe, M.Inoue
    • Journal Title

      Industrial and Engineering Chemistry, Research (印刷中)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Synthesis of γ-Ga_2O_3-Al_2O_3 Solid Solutions by the Glycothermal Method

    • Author(s)
      M.Takahashi, N.Inoue, T.Nakatani, T.Takeguchi, S.Iwamoto, M.Inoue, T.Watanabe
    • Journal Title

      Journal of American Ceramic Society (印刷中)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Effect of Modification by alkali on the γ-Ga_2O_3-Al_2O_3 Mixed Oxides by the Glycothermal Method

    • Author(s)
      M.Takahashi, T.Nakatani, S.Iwamoto, T.Watanabe, M.Inoue
    • Journal Title

      Journal of Physics : Condensed Matter (印刷中)

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Synthesis of γ-Ga_2O_3-Al_2O_3 Binary Oxide by the Glycothermal Method and Its Catalytic Performance for SCR of NO with Methane

    • Author(s)
      Masaru Takahashi, Shinji Iwamoto, Masashi Inoue
    • Journal Title

      Proceedings of 13^<th> International Congress on Catalysis P6-106(印刷中)

    • Related Report
      2004 Annual Research Report
  • [Presentation] The Synthesis of γ-Ga_2O_3-Al_2O_3 Binary Oxide by the Glycothermal Method and Its Catalytic Performance2004

    • Author(s)
      M.Takahashi, S.Iwamoto, K.Kagawa, M.Inoue
    • Organizer
      13th International Conference on Catalysis
    • Place of Presentation
      Paris
    • Year and Date
      2004-07-15
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Presentation] The Synthesis of y-Ga_20_3-Al_20_3 Binary Oxide by the Glycothermal Method and Its Catalytic Performance2004

    • Author(s)
      M. Takahashi, S. Iwamoto, K. Kagawa, M. Inoue
    • Organizer
      13th International Conference on Catalysis
    • Place of Presentation
      Paris
    • Year and Date
      2004-07-15
    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Book] Chemical Processing of Metal Oxides2005

    • Author(s)
      Masashi Inoue(分担執筆)
    • Total Pages
      42
    • Publisher
      Taylor & Francis
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Book] Chemical Processing of Ceramics : Chapter 2,"Solvothermal Synthesis"(B.Lee, S.Komarneni編)2005

    • Author(s)
      M.Inoue
    • Total Pages
      43
    • Publisher
      Taylor & Francis, London
    • Related Report
      2005 Annual Research Report
  • [Publications] Masashi INOUE: "Glycothermal synthesis of metal oxides"J.Phys.Condens.Matter. 16. S1291-S1303 (2004)

    • Related Report
      2003 Annual Research Report

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

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