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Easy-separable magnetic nanoparticle-supported Pd catalysts: Kinetics, stability and catalyst re-use

机译:易分离的磁性纳米颗粒负载Pd催化剂:动力学,稳定性和催化剂重复使用

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摘要

A series of novel palladium-based catalysts supported on magnetic nanoparticles with diameters of 7–17 nm have been prepared and evaluated in C–C coupling, hydrogenation and amination reactions. One type of catalyst used palladium complexes containing phosphine and/or acetate ligands for applications in Suzuki and Heck reactions. The second type consisted of Pd(0)-functionalised magnetic cores for use in hydrogenation and C–C coupling. Each type was effective for a range of reactions and was easily recoverable from the reaction mixture due to the superparamagnetic behaviour of the support. Detailed rate studies, found to correspond to pseudo-first-order kinetics, were conducted to assist in determining the mechanism of the reactions and showed that, during Heck reactions, Pd leaching is critically dependent on the presence of the aryl halide. The catalysts were found to retain their activity for several cycles although the rate of reaction was markedly reduced on re-use.
机译:已经制备了一系列新型的钯基催化剂,负载在直径7-17 nm的磁性纳米粒子上,并进行了C-C偶联,氢化和胺化反应的评估。一种类型的催化剂使用包含膦和/或乙酸酯配体的钯配合物,用于Suzuki和Heck反应。第二种类型是用于氢化和CC偶联的Pd(0)-官能化磁芯。每种类型均对一系列反应有效,并且由于载体的超顺磁性行为,很容易从反应混合物中回收。进行了详细的速率研究,发现其与拟一级反应动力学相对应,以帮助确定反应机理,结果表明,在Heck反应过程中,Pd浸出关键取决于芳基卤化物的存在。尽管重复使用时反应速率明显降低,但发现催化剂可以保持其活性数个循环。

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