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Immobilization of palladium catalyst on magnetically separable polyurea nanosupport

机译:磁性可分离聚脲纳米载体上钯催化剂的固定化

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摘要

This work describes a method for preparing magnetic polyurea nanoparticles (PU NPs) and their utilization as a catalyst support. The method is based on entrapment of hydrophilic magnetic nanoparticles within the polyurea matrix. The synthetic process of these magnetic polyurea nanoparticles is based on oil-in-oil nanoemulsification of an organic polar phase comprised of N, N-dimethylacetamide (DMAc), 2,6-diaminopyridine and ionic liquid modified magnetite nanoparticles (MNPs-IL), in heptane containing a suitable surfactant. This was followed by interfacial polycondensation reaction between an isocyanate monomer, polymethylenepolyphenyl isocyanate (PAPI 27), and the amine monomer producing magnetically separable polyurea nanoparticles. Subsequently, these particles were employed as a catalyst nanosupport. Two catalytic systems based on the encapsulation of Pd(OAc)(2) within magnetic PU NPs or their adsorption on the surface of these particles were produced and subjected to hydrogenation reactions and selective hydrogenations of alpha,beta-unsaturated compounds. Pd(OAc)(2) adsorbed on the surface of the magnetic PU NPs demonstrated high catalytic activity and selectivity, which was superior to the conventional catalyst Pd/C or palladium nanoparticles supported directly on the surface of magnetite nanoparticles. The catalyst was easily recovered from the reaction mixture by applying an external magnetic field and recycled over five times without observing any significant loss in its catalytic efficiency.
机译:这项工作描述了一种制备磁性聚脲纳米颗粒(PU NPs)的方法及其作为催化剂载体的用途。该方法基于将亲水性磁性纳米颗粒截留在聚脲基质中。这些磁性聚脲纳米粒子的合成过程基于油极性纳米乳化,该油性油相由N,N-二甲基乙酰胺(DMAc),2,6-二氨基吡啶和离子液体改性磁铁矿纳米颗粒(MNPs-IL)组成,在庚烷中含有合适的表面活性剂。随后进行异氰酸酯单体,聚亚甲基多苯基异氰酸酯(PAPI 27)和胺单体之间的界面缩聚反应,从而产生可磁分离的聚脲纳米粒子。随后,将这些颗粒用作催化剂纳米载体。基于Pd(OAc)(2)在磁性PU NP中的封装或它们在这些颗粒表面的吸附,建立了两个催化体系,并进行了氢化反应和α,β-不饱和化合物的选择性氢化。吸附在磁性PU NPs表面的Pd(OAc)(2)具有较高的催化活性和选择性,优于直接负载在磁铁矿纳米颗粒表面的常规催化剂Pd / C或钯纳米颗粒。通过施加外部磁场可以容易地从反应混合物中回收催化剂,并循环五次,而没有观察到其催化效率的任何重大损失。

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