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1999 Fiscal Year Final Research Report Summary

Study of Catalytic Conversion of Organosilicon Compounds

Research Project

Project/Area Number 09450298
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 InstitutionEhima University

Principal Investigator

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

Co-Investigator(Kenkyū-buntansha) 大川 政志  愛媛大学, 工学部, 助手 (00274340)
Project Period (FY) 1997 – 1999
Keywordsorganosilane / solid superacid / ketone / solid acid / isotopic tracer / hydrosilylation
Research Abstract

Both in laboratories and industries, reactions of organosilane are usually performed in a homogeneous liquid phase using metal halides and transition metal complexes. The development of fundamental chemistries of Si compounds in heterogeneous catalysis is quite attractive and important challenge. Hence the activation process and the catalytic conversion of alkylsilanes were examined.
1. On the initiation step of alkylsilane activation as a model of hydrocarbon activation
Catalytic conversion of hydrocarbons in superacidic media is initiated by proton addition yielding a 3c-2e or 5-coordinated intermediate, which decomposes to carbenium ion and hydrogen or alkanes such as methane. NMR and XPS have directly evidenced the existences of such intermediates and the following process. On solid surface like solid acid, it is hard to obtain them since superacidic solid acid is rare to activate saturated hydrocarbons under mild condition. Si-H in organosilane is more active than C-H bond in alkane … More s. Thus We examined the initiation step of alkylsilanes from the hydrogen evolution and the HD content when the silane was contact With deuterated solid acid. As a result, we found (1) hydrogen evolution occurs around room temperature, (2) amount of hydrogen molecule was in the order of μmol g-1, and (3) there are two types of hydrogen evolution process, one is ionic and the other is non- ionic.
2. Catalytic hydrosilylation of aliphatic ketones
Title reaction was examined by using triethylsilane (E3) and diethylsilane (E2) with diethylketone and cyclohexanone at room temperature in a glass batch type reactor. The catalyst was CaO and Al2O3. We obtained silylether from E2 and ketones as a single product in 70-90 % yield after 20-40 h reaction. By-products were the products of aldol condensation of ketone itself. By decreasing the E2/ketone ratio, the yield decreased which indicates a strong interaction of ketones with the catalyst surface. E3 was totally inactive, probably because of the steric hindrance on solid surface.
These results are the first finding of the heterogeneous catalytic conversion of organosilicone compounds in the world. Less

  • Research Products

    (10 results)

All Other

All Publications (10 results)

  • [Publications] 山口力: "金属酸化物へのアニオン添加による強酸、強塩基の発生"触媒調製の進歩. 53-59 (2000)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] T.Yamaguchi: "Development of a New Solid Base Catalyst and its Application to Fine Chemicals Synthesis"Proc.3rd.Tokyo Conf.Adv.Catal.Sc.Tech.(TOCAT3). 334-335 (1998)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] T.Yamaguchi: "Supported K-salts as a New Solid Base Catalyst"Abstr.Intern.Symp.on Acid-Base Catalysis III. 43-44 (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] T.Yamaguchi: "Solid Acid Catalyzed Disproportionation and Alkylation of Alkylsilanes"Stud.Surf.Sc.Catal.. 108. 617-624 (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] T.Yamacuchi: "Supported K-salts as New solid Base Catalyst"Chem.Lett.. 989-990 (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] 山口力: "固体超強酸、固体超強塩基、酸塩基両機能触媒"ペトロテック. 20. 60-65 (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [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"Proc.3rd.Tokyo Conf.Adv.Catal.Sc.Tech.(TOCAT 3) Tokyo. 334-335 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] T. Yamaguchi, J.-H.Zhu, Y. Wang, M. Komatsu, M. Ookawa: "Supported K-salts as a New Solid Base Catalyst"Abstr.Intern.Symp. On Acid-Base Catalysis III, Rolduc. 43-44 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] T. Yamaguchi, T. Yamada, M. Shibata, T. Tsuneki, M. Ookawa: "Solid Acid Catalyzed Disproportionation and Alkylation of Alkylsilanes"Stud.Surf.Sc.Catal.. 108. 617-624 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] T. Yamaguchi, J.-H. Zhu, Y. Wang, M. Komatsu, M. Ookawa: "Supported K-salts as New Solid Base Catalyst"Chem.Lett.. 989-990 (1997)

    • Description
      「研究成果報告書概要(欧文)」より

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Published: 2001-10-23  

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