导　　师： 万伯顺

学科专业： 070303

授予学位： 硕士

作　　者： ;

机构地区： 中国科学院研究生院

摘　　要： Suzuki 交叉偶联反应是构建Csp~2-Csp~2键重要的合成方法学之一,其产物联苯类化合物在作为药物前体、聚合物、材料、液晶及配体等领域有着广泛的应用。近年来各类高效催化体系的报道为该反应的应用与发展提供了更为广阔的空间。基于环境考虑以及为简化后处理、贵金属催化剂的回收使用,多相、高分子负载催化剂以及水溶液体系的催化剂正迅速发展。 在本论文中,我们通过原位加入第二种金属盐调节高分子负载Pd 催化Suzuki 反应,用组合平行法/(即高通量筛选实验High-throughput experiment /)快速对多种金属盐和碱进行了考察筛选,从中发现Ni, Cu, Fe 等过渡金属盐能有效地促进Pd催化Suzuki反应,其中以Ni盐效果最好,从而取得了高效的Pd//PVP+Ni 双金属催化体系。该反应体系适用于各类芳香溴代化合物与芳基硼酸的催化Suzuki 偶联反应,而且反应可以在水溶液中顺利进行。对本文的双金属催化机理进行了探讨。 Suzuki coupling reaction is one of the most important methodology for construction ofcarbon-carbon bond. The product of Suzuki coupling was widely used as precursors forpharmaceuticals, polymers, materials, liquid crystals, and ligands. In recent years, the report ofvarious highly efficient catalyst systems for Suzuki coupling provided more spacious prospect forits development and application. Owing to increasing environmental concerns, simplifying thehandling works and to recycling the noble metals, the heterogeneous catalyst andpolymer-bounded catalyst such as aqueous catalyst systems are presently undergoing veryrapidly. In this paper, the activity of polymer-supported palladium was improved by introducing thesecond transition metal salt in situ for catalytic Suzuki coupling, and the effect of varioustransition metals salts and bases were investigated by High-throughput experiment /(HTE/) method.As a result, we developed a ligand-free, simple, readily available and highly effectivePd//PVP+Ni bimetallic catalyst system for Suzuki coupling reaction. The protocol is applicable tomany representative aryl bromide substrates bearing different functional groups with good yields.Moreover, in aqueous media, the Suzuki coupling reaction can effectively be carried out with thiscatalyst system. The mechanism of the bimetallic catalytic reaction was discussed.

关 键 词： 反应 组合催化 高分子负载催化剂 双金属催化

分 类 号： [O643.32]

领　　域： [理学] [理学]