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负载 Pd NPs 的碳化纤维素微球作为 p-硝基苯酚还原和 Suzuki-Miyaura 偶联反应的催化剂。

Carbonized cellulose microspheres loaded with Pd NPs as catalyst in p-nitrophenol reduction and Suzuki-Miyaura coupling reaction.

机构信息

School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, LiuFang Campus, No.206, Guanggu 1st road, Donghu New & High Technology Development Zone, Wuhan 430205, Hubei Province, PR China.

Department of Medical Research Center, the First Affiliated Hospital of Ningbo University, Ningbo 315010, PR China.

出版信息

Int J Biol Macromol. 2024 Jun;269(Pt 2):131904. doi: 10.1016/j.ijbiomac.2024.131904. Epub 2024 Apr 28.

Abstract

Catalytic reduction of p-nitrophenol is usually carried out using transition metal nanoparticles such as gold, palladium, silver, and copper, especially palladium nanoparticles (Pd NPs), which are characterized by fast reaction rate, high turnover frequency, good selectivity, and high yield. However, the aggregation and precipitation of the metals lead to the decomposition of the catalyst, which results in a significant reduction of the catalytic activity. Therefore, the preparation of homogeneous stabilized palladium nanoparticles catalysts has been widely studied. Stabilized palladium nanoparticles mainly use synthetic polymers. Cellulose microspheres, as a natural polymer material with low-cost and porous fiber network structure, are excellent carriers for stabilizing metal nanoparticles. Cellulose microspheres impregnated with palladium metal nanoparticles were carbonized to have a larger specific surface area and highly dispersed palladium nanoparticles, which exhibited excellent catalytic activity in the catalytic reduction of p-nitrophenol. In this work, the cellulose carbon-based microspheres palladium (Pd@CCM) catalysts were designed and characterized by SEM, TEM, EDS, XRD, FTIR, XPS, TGA, BET, and so on. Furthermore, the catalytic performance of Pd@CCM catalysts was investigated via p-nitrophenol reduction, which showed high catalytic activity. This catalyst also exhibited excellent catalytic performance in the Suzuki-Miyaura coupling reaction. Linking aromatic monomer and benzene through Suzuki-Miyaura coupling was presented as an effective route to obtaining biaryls, and the synthesis method is low-cost and simple. In addition, Pd@CCM showed desirable recyclability while maintaining its catalytic activity even after five recycles. This work is highly suggestive of the design and application of the heterogeneous catalyst.

摘要

通常使用过渡金属纳米粒子(如金、钯、银和铜),特别是钯纳米粒子(Pd NPs),来催化还原对硝基苯酚。这些纳米粒子具有反应速率快、转化率高、选择性好、产率高等特点。然而,金属的聚集和沉淀会导致催化剂分解,从而显著降低催化活性。因此,制备均相稳定的钯纳米粒子催化剂已得到广泛研究。稳定化的钯纳米粒子主要使用合成聚合物。纤维素微球作为一种具有低成本和多孔纤维网络结构的天然聚合物材料,是稳定金属纳米粒子的优良载体。用钯金属纳米粒子浸渍的纤维素微球碳化后具有更大的比表面积和高度分散的钯纳米粒子,在催化还原对硝基苯酚中表现出优异的催化活性。在这项工作中,通过 SEM、TEM、EDS、XRD、FTIR、XPS、TGA、BET 等手段对纤维素基碳微球钯(Pd@CCM)催化剂进行了设计和表征。此外,还通过对硝基苯酚还原反应考察了 Pd@CCM 催化剂的催化性能,结果表明其具有高催化活性。该催化剂在 Suzuki-Miyaura 偶联反应中也表现出了优异的催化性能。通过 Suzuki-Miyaura 偶联将芳基单体和苯连接起来是获得联苯的有效途径,且该合成方法成本低、简单。此外,Pd@CCM 在保持催化活性的情况下,即使经过五次循环仍具有良好的可回收性。这项工作为异相催化剂的设计和应用提供了重要的参考。

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