Silyl-transition-metal complexes : Synthesis, Structure, Reactivity, and Application to Catalysis

甲硅烷基过渡金属配合物:合成、结构、反应性及其催化应用

基本信息

项目摘要

The reaction of bidentate and tridentate silyl ligand precursor hydrosilanes with group 10 transition-metal complexes was studied for the advancement of basic chemistry of silicon-transition-metal complexes and for the development of efficient catalysts for Si-Si bond forming reactions. The results showed that the chemistry of silicon-group 10 transition-metal complexes has a diversity beyond our expectation. Also we obtained important information for the development of catalysts for Si-Si bond forming reaction. The major results of this research are listed below.It was clarified that the reaction of the tridentate hydrosilane, (2-SiH_3C_6H_4)_2SiH_2,with group 10 transition-metal complexes provided diverse range of products depended on the metals and the steric hindrance of the ligands. We for the first time succeeded in the isolation and structure determination of a silylnickel complex that has a Ni^<IV>(H)(Si)_3 structure in the solid state while η^2-(Si-H)Ni structure in solution.・We succeeded in the isolation and structure determination of trinuclear and tetranuclear Pd complexes having Pd centers ligated by five Si atoms. This is the first example of Pd complex with a Pd center ligated by five formally anionic ligands.・The first example of Pt complex with cyclodisiloxane moiety was obtained by the reaction of the bidentate hydrosilane with a Pt(0) phosphine complex.・It was clarified that the reaction of the bidentate and the tridentate hydrosilanes with group 10 transition metal phosphine complexes was highly affected by the steric hindrance of phosphine ligands and of the hydrosilanes. If the steric hindrance is small, multinuclear complexes and high formal oxidation state complexes are easily formed. On the other hand, if the steric hindrance is severe, Si-Si bond forming reaction often takes place. This finding provides important information for the development of efficient catalysts for a Si-Si bond forming reaction.
研究了二齿和三齿硅基配体前体氢硅烷与第10族过渡金属配合物的反应,以推进硅-过渡金属配合物的基础化学,并为Si-Si键形成反应开发有效的催化剂。结果表明,硅-第10族过渡金属配合物的化学性质具有超出预期的多样性。我们还为硅-硅键形成反应催化剂的开发获得了重要信息。本研究的主要结果如下:(2-SiH_3C_6H_4)_2SiH_2与第10族过渡金属配合物的反应,根据金属的种类和配体的空间位阻,得到了不同的产物。本文首次成功地分离和测定了一种硅基镍配合物的结构,该配合物在固态下具有Ni^<IV>(H)(Si)_3结构,而在溶液中具有η^2-(Si-H)Ni结构。我们成功地分离和结构测定的三核和四核钯配合物的钯中心的五个硅原子连接。这是Pd络合物的第一个例子,其中Pd中心被五个形式上的阴离子配体连接。·具有环二硅氧烷部分的Pt络合物的第一个实例通过双齿氢硅烷与Pt(0)膦络合物的反应获得。已阐明,二齿和三齿氢硅烷与第10族过渡金属膦络合物的反应受到膦配体和氢硅烷的空间位阻的高度影响。如果空间位阻小,则容易形成多核络合物和高形式氧化态络合物。另一方面,如果空间位阻严重,则经常发生Si-Si键形成反应。这一发现提供了重要的信息,有效的催化剂的Si-Si键形成反应的发展。

项目成果

期刊论文数量(13)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
ケイ素-10族遷移金属錯体の化学
硅-10族过渡金属配合物的化学
  • DOI:
  • 发表时间:
    2004
  • 期刊:
  • 影响因子:
    0
  • 作者:
    仲村 允;藤岡岳史;坂本英文;木村恵一;島田 茂
  • 通讯作者:
    島田 茂
A PtIII2Si2 Four-Membered Cycle and a Dinuclear Platinum Complex Bridged by a Cyclodisiloxane Ring
  • DOI:
    10.1021/om0604019
  • 发表时间:
    2006-06
  • 期刊:
  • 影响因子:
    2.8
  • 作者:
    S. Shimada;Yonghua Li;M. Rao;Masato Tanaka
  • 通讯作者:
    S. Shimada;Yonghua Li;M. Rao;Masato Tanaka
Group 10 transition-metal complexes with metal-silicon bonds derived from 1, 2-disilylbenznes and bis (2-si lylphenyl) silane
衍生自 1, 2-二甲硅烷基苯和双 (2-甲硅烷基苯基) 硅烷的具有金属-硅键的第 10 族过渡金属络合物
  • DOI:
  • 发表时间:
    2006
  • 期刊:
  • 影响因子:
    0
  • 作者:
    S.Shimada;M.Tanaka
  • 通讯作者:
    M.Tanaka
Group 10 transition-metal complexes with metal-silicon bonds derived from 1,2-disilylbenzenes and bis(2-silylphenyl)silane
  • DOI:
    10.1016/j.ccr.2005.12.010
  • 发表时间:
    2006-05
  • 期刊:
  • 影响因子:
    20.6
  • 作者:
    S. Shimada;Masato Tanaka
  • 通讯作者:
    S. Shimada;Masato Tanaka
Reaction of 1-(Dimethylsilyl)-2-silylbenzene with Platinum(0) Phosphine Complexes
  • DOI:
    10.1021/om050498j
  • 发表时间:
    2005-10
  • 期刊:
  • 影响因子:
    2.8
  • 作者:
    S. Shimada;M. Rao;‡. Li;Masato Tanaka
  • 通讯作者:
    S. Shimada;M. Rao;‡. Li;Masato Tanaka
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SHIMADA Shigeru其他文献

SHIMADA Shigeru的其他文献

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{{ truncateString('SHIMADA Shigeru', 18)}}的其他基金

Synthesis of Transition-metal-encapsulating Silicon Cages
过渡金属封装硅笼的合成
  • 批准号:
    23655058
  • 财政年份:
    2011
  • 资助金额:
    $ 9.47万
  • 项目类别:
    Grant-in-Aid for Challenging Exploratory Research
Context Awareness Service System by Mobile Video Database Retrieval and Mining
移动视频数据库检索与挖掘的情境感知服务系统
  • 批准号:
    20500098
  • 财政年份:
    2008
  • 资助金额:
    $ 9.47万
  • 项目类别:
    Grant-in-Aid for Scientific Research (C)
A developmental study on teaching materials concerning connection between high school mathematics and college mathematics
高中数学与大学数学衔接教材的开发研究
  • 批准号:
    58880032
  • 财政年份:
    1983
  • 资助金额:
    $ 9.47万
  • 项目类别:
    Grant-in-Aid for Developmental Scientific Research

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铂族金属配合物溶解度的研究及钯选择性沉淀剂的开发
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  • 批准号:
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Asymmetric Hetero-Dinuclear Catalysis via Cooperation of Platinum(II) and Palladium(II) for the Stereoselective Formation of Quaternary Stereocenters
铂(II)和钯(II)合作的不对称异双核催化立体选择性形成四元立构中心
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    Research Grants
Molecular Activation on the Basis of the Palladium and Platinum Mixed Multninuclear Complexes
基于钯和铂混合多核配合物的分子活化
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    25410061
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Square planar platinum and palladium complexes of tridentate carbazole-based ligands as SPECT agents
作为 SPECT 试剂的三齿咔唑基配体的方形平面铂和钯配合物
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    436734-2012
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Pathfinding research for marine geochemistry of palladium, platinum and gold
钯、铂、金海洋地球化学探路研究
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    22651006
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    2010
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铂、钯和铑的地球微生物学和(生物)地球化学
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Novel Platinum and Palladium Reactions Relevant to Hydrocarbon Functionalization
与碳氢化合物官能化相关的新型铂和钯反应
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