Development of novel highly active ROMP catalysts based on Group 5 transition metals
基于第5族过渡金属的新型高活性ROMP催化剂的开发
基本信息
- 批准号:18550110
- 负责人:
- 金额:$ 2.63万
- 依托单位:
- 依托单位国家:日本
- 项目类别:Grant-in-Aid for Scientific Research (C)
- 财政年份:2006
- 资助国家:日本
- 起止时间:2006 至 2007
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
Pentavalent tantalum and niobium complexes with aryloxy ligands, (2,6-R_2C_6H_3O)MCl_4 (M=Ta, Nb; R=H, Me, ^iPr, Ph), were prepared, and their catalytic behaviors for the ring-opening metathesis polymerization (ROMP) of norbornene (NBE) were systematically studied in the presence of alkylaluminum cocatalysts, R'_3Al (R'=Me, Et, ^iBu). Tantalum complexes were found to show very high activity for the ROMP of NBE in combination with ^iBu_3Al to give high-molecular-weight polymers (M_n>10^5) and relatively narrow molecular weight distributions (M_w/M_n〜2), implying that these are single-site catalysts. With increasing the bulkiness of the ligand, the tantalum catalyst systems became less active. In sharp contrast, the aryloxyniobium complexes were revealed to exhibit very high activity upon activation with Me_3Al to give high-molecular weight polymers. With increasing the bulkiness of the ligand, the activity of the niobium catalyst systems increased. We also studied synthesis of pentavalent tantalum and niobium complexes having catecholato, tropolonato, hinokitiolato, biphenolato, and binaphtolato ligands, and their catalyses for the ROMP of NBE in the presence of trialkylaluminum as a cocatalyst. Among those complexes, the tantalum complexes also showed high activity upon activation with ^iBu_3Al for ROMP of NBE. In contrast, the biphenolato and binaphtholato complexes of niobium were effectively activated with Me_3Al rather than with ^iBu_3Al. The polymers obtained with those complexes had high molecular weight (M_n>10^5) and relatively narrow molecular weight distributions (M_w/M_n〜2) implying that these are single-site catalysts. These findings will contribute to future development of ROMP catalysts.
合成了五价钽、铌芳氧基配合物(2,6-R_2C_6H_3O)MCl_4(M=Ta,Nb; R=H,Me,^iPr,Ph),并系统研究了它们在烷基铝助催化剂R '_3Al(R'= Me,Et,^iBu)存在下对异戊二烯(NBE)开环易位聚合(ROMP)的催化性能。结果表明,钽配合物与^iBu_3Al配合时,对NBE的开环聚合反应具有很高的催化活性,可得到高分子量聚合物(Mn>10^5)和相对较窄的分子量分布(Mw/Mn> 2),表明它们是单活性中心催化剂。随着配体体积的增加,钽催化剂体系的活性降低。与此形成鲜明对比的是,芳氧基铌配合物显示出非常高的活性时,用Me_3Al活化,得到高分子量的聚合物。随着配体体积的增加,铌催化剂体系的活性增加。我们还研究了以邻苯二酚、托洛酮、扁柏酚、双酚和联萘酚为配体的五价钽和铌配合物的合成,以及它们在三烷基铝助催化剂存在下对NBE的ROMP反应的催化作用。在这些配合物中,钽配合物也表现出较高的活性时,与^iBu_3Al的活化NBE的ROMP。相比之下,铌的双酚和联萘酚络合物被Me_3Al而不是^iBu_3Al有效活化。用这些配合物得到的聚合物具有高的分子量(Mn>10^5)和相对窄的分子量分布(Mw/Mn> 2),这意味着它们是单活性中心催化剂。这些发现将有助于ROMP催化剂的未来发展。
项目成果
期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Ring-opening metathesis polymerization of norbornene catalyzed by tantalum and niobium complexes with chelating O-donor ligands
钽铌配合物与螯合 O 供体配体催化降冰片烯的开环复分解聚合
- DOI:
- 发表时间:2008
- 期刊:
- 影响因子:0
- 作者:Yuushou Nakayama;Naoaki Maeda;Hajime Yasuda;Takeshi Shiono
- 通讯作者:Takeshi Shiono
Ring-opening metathesis polymerization of norbornene catalyzed by group 5 transition metal complexes bearing phenoxy ligands
苯氧基配体5族过渡金属配合物催化降冰片烯开环复分解聚合
- DOI:
- 发表时间:2006
- 期刊:
- 影响因子:0
- 作者:Masaya;Tanimoto;Yuushou;Nakayama;Takeshi;Shiono
- 通讯作者:Shiono
Synthosis of bis(imino)pyridine complexes of group 5 metals and their catalysis for polymerization of ethylcne and norbornene
5族金属双(亚氨基)吡啶配合物的合成及其催化乙烯和降冰片烯聚合
- DOI:
- 发表时间:2006
- 期刊:
- 影响因子:0
- 作者:Yuushou;Nakayama;Masaya;Tanimoto;Takeshi;Shiono;Yuushou Nakayama;Yuushou Nakayama
- 通讯作者:Yuushou Nakayama
Effect of cocatalysts on catalytic activities of tantalum-and niobium-based catalysts for ring-opening metathesis polymerization of norbornene
助催化剂对钽铌基催化剂降冰片烯开环易位聚合催化活性的影响
- DOI:
- 发表时间:2007
- 期刊:
- 影响因子:0
- 作者:Yuushou;Nakayama;Masaya;Tanimoto;Takeshi;Shiono
- 通讯作者:Shiono
Effect of Cocatalysts on the Catalytic Activities of Tantalum-and Niobium-Based Catalysts for Ring -Opening Metathesis Polymeriz ation of Norbornene
助催化剂对钽铌基催化剂降冰片烯开环易位聚合催化活性的影响
- DOI:
- 发表时间:2007
- 期刊:
- 影响因子:0
- 作者:Yuushou;Nakayama;Masaya;Tanimoto;Takeshi;Shiono;Yuushou Nakayama
- 通讯作者:Yuushou Nakayama
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NAKAYAMA Yuushou其他文献
NAKAYAMA Yuushou的其他文献
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{{ truncateString('NAKAYAMA Yuushou', 18)}}的其他基金
Development of new biodegradable cationic ionomers
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- 批准号:
24550136 - 财政年份:2012
- 资助金额:
$ 2.63万 - 项目类别:
Grant-in-Aid for Scientific Research (C)
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