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Synthesis of novel transition metal dinuclear complex catalyst and application to organic synthesis

新型过渡金属双核配合物催化剂的合成及其在有机合成中的应用

基本信息

批准号：
14550816
负责人：
INOUE Yoshio
金额：
$ 2.24万
依托单位：
Tohoku University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2002
资助国家：
日本
起止时间：
2002 至 2004
项目状态：
已结题

项目摘要

We have exploited a novel tetradentate ligand (Hdpfam) containing nitrogen and phosphorus donor atoms. Several dinuclear complexes (M_2Ar_2(η-X)(η-dpfam), M=Pd, Pt, Rh) can be synthesized using this ligand. Development of catalytic reactions utilizing the dinuclear complexes mediated only by dinuclear system has been studied and the following results are obtained.1.Hydrosilylation of alkynes catalyzed by dinuclear platinum complexDinuclear platinum hydride complex Pt_2Tbl_2(η-H)(η-dpfam)) obtained by treatment of the chloride bridged platinum dinuclear complex with sodium borohydride was found to be a good catalyst for the hydrosilylation of alkynes.2.Activation of C-H bond of aromatic compounds by dinuclear palladium complexesDinuclear palladium complexes were found active far hydroarylation of alkynes activating the C-H bond of an aromatic ring which was usually regarded inert. Elucidation of the reaction mechanism uncovered that the reaction proceeds with direct C-H bond activation by palladium center.3.Activation of C-H bond of alkenesDinuclear palladium complexes were found active for hydroalkenylation of alkynes activating the C-H bond of an alkene double bond which was usually regarded inert.4.Suzuki-Miyaura reaction catalyzed by dinuclear palladium complexDinuclear palladium complexes catalyzed the Suzuki-miyaura reaction in benzene solvent to give a cine product together with the normal one.5.Double carbonylation catalyzed by dinuclear palladium complexDinuclear palladium complex was found to be an active catalyst for the double carbonylation of iodobenzene with diethylamine.

我们已经开发了一种新的四齿配体（Hdpfam）含有氮和磷供体原子。用该配体可以合成出几种双核配合物（M_2Ar_2（η-X）（η-dpfam），M=Pd，Pt，Rh）。本文研究了双核配合物催化反应的发展，得到以下结果：1.双核铂配合物催化炔的硅氢加成反应用硼氢化钠处理氯桥铂双核配合物得到的催化剂是一种很好的硅氢加成反应的催化剂。2.双核钯配合物对芳香化合物C-H键的活化双核钯配合物对炔的氢芳基化反应具有活性，活化了通常被认为是惰性的芳香环上的C-H键。4.双核钯配合物催化的Suzuki-Miyaura反应，研究了双核钯配合物催化的Suzuki-Miyaura反应的机理，结果表明，双核钯配合物催化的Suzuki-Miyaura反应是一种新型的催化剂。5.双核钯配合物催化的双羰基化双核钯配合物是碘苯与二乙胺双羰基化反应的活性催化剂。