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Development of Solid Superbase by Controlled Oxygen Anion Generation

Research Project

Project/Area Number 12650778
Research Category

Grant-in-Aid for Scientific Research (C)

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

Principal Investigator

YAMAGUCHI Tsutomu  Ehime University, Faculty of Engineering, Department of Applied Chemistry, Professor, 工学部, 教授 (10000861)

Co-Investigator(Kenkyū-buntansha) OOKAWA Masashi  Ehime University, Faculty of Engineering, Department of Applied Chemistry, Instructor, 工学部, 助手 (00274340)
MIYAZAKI Takafumi  Ehime University, Faculty of Engineering, Department of Applied Chemistry, Associate Professor, 工学部, 助教授 (70260156)
Project Period (FY) 2000 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥3,300,000 (Direct Cost: ¥3,300,000)
Fiscal Year 2001: ¥1,400,000 (Direct Cost: ¥1,400,000)
Fiscal Year 2000: ¥1,900,000 (Direct Cost: ¥1,900,000)
Keywordssolid base / alkali metal salts / olefin isomerization / green chemistry
Research Abstract

1. A highly basic solid catalyst was obtained by dispersing metal salts over supports at the surface density of 10 - 15 x 10^<18> K^+ ions m^<-2> and activating them at proper temperature in an inert atmosphere. Metal salts can be the nitrate or carbonate of group 1 elements. Effective supports were alumina and zirconia; silica and titania are ineffective.
2. The catalyst exhibited high activity in the isomerizations of cis-but-2-ene, 3-methyl-but-l-ene, propa-1,2-diene and α-pinene, and the isomerization/dehydrogenation of cyclohexadiene to benzene, cyclohexene and hydrogen, and of limonene to p-cymene
3. From TPD and IR/Raman spectroscopy, it was found that mounted metal salts exist as both an agglomerated phase when the surface density is high and an ion-separated phase when the surface density is low. The former decomposes at the temperature close to its own decomposition temperature, while the latter decomposes far below the decomposition temperature and was attributed to the anion decomposition that may be free from its counter cation.
4. The generation of basic property closely relates to the anion decomposition. NO_3^- decomposes to NO_2 + O^- and CO_2 decomposes to CO_2 + O^<2->. It is suspected that the liberated oxygen anion(s) constitutes basic centers.
5. It is speculated that liberated oxygen anions can be discriminated from the anions of metal oxide supports in case of alumina and zirconia, while can not on titania support. Metal salts can only exist as agglomerated phase on silica support that was confirmed by XRD. Effectiveness of support could be the difference of the discrimination ability of liberated oxygen anions from those of supports. The loss of basicity at elevated temperatures could be attributed to the leveling of both oxygen anions.

Report

(3 results)
  • 2001 Annual Research Report   Final Research Report Summary
  • 2000 Annual Research Report
  • Research Products

    (23 results)

All Other

All Publications (23 results)

  • [Publications] T.Yamaguchi, Y.Wang, M.Komatsu, M.Ookawa: "New Solid Base Derived from Supported Metal Nitrates and Carbonates"Catal. Survey from Japan. 5. 81-89 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Yamaguchi: "Alkane Isomerization and Acidity Assessment on Sulfated ZrO_2"Applied Catalysis. 222. 237-246 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] M.Oookawa, Y.Yogoro, T.Yamaguchi, K.Kawamura: "X-Ray Diffraction Analysis of Ordered Mesoporous Silica"Studies of Surface Science and Catalysis. 135. 135 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Yamaguchi, N.Kasuya: "On the hydrogen liberation from alkylsilane with deuterated solid acid as a model of hydrocarbon activation"Proceedings of 12th International Congress on Catalysis. (CD R). 072 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Ishizuka, H.Kabashima, T.Yamaguchi, K.Tanabe, H.Hattori: "Initial Step of Flue Gas Desulfurization -An IR Study of the Reaction of SO_2 with NOx on CaO-"Environmental Science and Technology. 34. 2799-2803 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y.Wang, M.Komatsu, T.Yokota, M.Mano, M.Ookawa, T.Yamaguchi: "Development of a New Solid Base Catalyst and its Application to Fine Chemicals Synthesis"Studies of Surface Science and Catalysis. 121. 334-335 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] 山口 力 他: "触媒調整の進歩"触媒調製化学振興会編、触媒学会. 107 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Yamaguchi and M. Ookawa: "New Solid Base Derived from supported Metal Nitrates and Carbonates"Catal. Survey from Japan. 5. 81-89 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Yamaguchi: "Alkane Isomerization and Acidity Assessment on Sulfated ZrO_2"Appl. Catal.. 222. 237-246 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] M. Ookawa, Y. Yogoro, T. Yamaguchi, and K. Kawamura: "X-Ray Diffraction Analysis of Ordered Mesoporous Silica"Stud. Surf. Sci. Catal.. 135. 198 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Yamaguchi and N. Kasuya: "On the hydrogen liberation from alkylsilane with deuterated solid acid as a model of hydrocarbon activation"Proc. Intern. Congr. Catal., Granada. (CD R072). (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Ishizuka, H. Kabashima, T. Yamaguchi, K. Tanabe, H. Hattori: "Initial Step of Flue Gas Desulfurizaion - An IR Study of the Reaction of SO_2 with NOx on CaO -"Environmental Science and Technology. 34. 2799-2803 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Y. Wang, M. Komatsu, T. Yokota, M. Mano, M. Ookawa, and T. Yamaguchi: "Development of a New Solid Base Catalyst and its Application to Fine chemicals Synthesis"Stud. Surf. Sci. Catal.. 121. 334-335 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Yamaguchi: "Generation of Strong Acidity and basicity by Anion Introduction on Metal Oxides, Progress in Catalyst Preparation"Promotion of Catalyst Preparation, catalysis Society of Japan. 53-59 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Yamaguchi, Y.Wang, M.Komatsu, M.Ookawa: "New Solid Base Derived from Supported Metal Nitrates and Carbonates"Catal. Survey from Japan. 5. 81-89 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Yamaguchi: "Alkane Isomerization and Acidity Assessment in Sulfated ZrO_2"Applied Catalysis. 222. 237-246 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] M.Oookawa, Y.Yogoro, T.Yamaguchi, K.Kawamura: "X-Ray Diffraction Analysis of Ordered Mesoporous Silica"Studies of Surface Science and Catalysis. 135. 135 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Yamaguchi, N.Kasuya: "On the hydrogen liberation from alkylsilane with deuterated solid acid as a model of hydrocarbon activation"Proceedings of 12th International Congress on Catalysis. CD R072 (2000)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Ishizuka, H.Kabashima, T.Yamaguchi, T.Tanabe, H.Hattori: "Initial Step of Flue Gas Desulfurization -An IR Study of the Reaction of SO_2 with NOx on CaO-"Environmental Science and Technology. 34. 2799-2803 (2000)

    • Related Report
      2001 Annual Research Report
  • [Publications] Y.Wang, M.Komatsu, T.Yokota, M.Mano, M.Ookawa, T.Yamaguchi: "Development of a New Solid Base Catalyst and its Application to Fine Chemical Synthesis"Studies of Surface Science and Catalysis. 121. 334-335 (1998)

    • Related Report
      2001 Annual Research Report
  • [Publications] 山口 力 他: "触媒調製の進歩"触媒調製化学振興会編、触媒学会. 107 (2000)

    • Related Report
      2001 Annual Research Report
  • [Publications] Tsutomu Yamaguchi: "On the hydrogen liberation from alkylsilane with deuterated solid acid as a model of hydrocarbon activation"Proc.12th Intern.Congr.Catal.,. CDR072 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Tsutomu Yamaguchi: "Initial Step of Flue Gas Desulfurization-An IR Study of the Reaction of SO_2 with Nox on CaO-"Environmental Science and Technology. 34. 2799-2803 (2000)

    • Related Report
      2000 Annual Research Report

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Published: 2000-04-01   Modified: 2016-04-21  

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