Beheshti Somaye, Motavalizadehkakhky Alireza, Zhiani Rahele, Nouri Seyed Mohammad Mahdi, Zahedi Ehsan
Department of Chemistry, Neyshabur Branch, Islamic Azad University, Neyshabur, Iran.
Avdanced Research Center for Chemistry, Biochemistry and Nanomaterial, Neyshabur Branch, Islamic Azad University, Neyshabur, Iran.
Sci Rep. 2024 May 25;14(1):11969. doi: 10.1038/s41598-024-62226-5.
Hercynite magnetic nanoparticles were produced through the co-precipitation of ferrous and aluminum cations. The surface of hercynite was respectively coated with silica, 2,4,6-trichloro-1,3,5-triazine, and 1H-pyrazole-3,5-dicarboxylic acid to provide a suitable substrate for Pd(II) loading, furnishing Pd@Her-TCT-PDA. Subsequently, the introduced Pd(II) was reduced to Pd(0) using NaBH. FT-IR, EDS, XRD, TGA, TEM and SEM images were the characteristic methods to prove the success of catalyst synthesis. The SEM image illustrated the particles with a nanosize of 25-50 nm and TEM image confirmed the presence of Pd nanoparticles with sizes lower than 2 nm. EDS elemental analysis of the catalyst proved the existence of Pd, Fe, and Al atoms along with the C, O, N, and Si atoms belong to the heterocyclic moieties. VSM analysis clarified a considerable drop in the magnetic properties of the hercynite core of the final catalyst due to its modified surface. TGA curve demonstrated that Pd@Her-TCT-PDA contains 20% organic content, attributed to the anchored heterocyclic ligands. Finally, Pd@Her-TCT-PDA was employed along with NaBH as a catalytic system to reduce completely the nitro group of aromatic compounds to their corresponding amines. The recyclability tests showed low drop in the catalytic activity of Pd@Her-TCT-PDA after third run with negligible leaching of Pd NPs.
通过亚铁离子和铝离子的共沉淀制备了铁尖晶石磁性纳米颗粒。分别用二氧化硅、2,4,6-三氯-1,3,5-三嗪和1H-吡唑-3,5-二羧酸包覆铁尖晶石表面,为负载Pd(II)提供合适的底物,从而制备出Pd@Her-TCT-PDA。随后,用硼氢化钠将引入的Pd(II)还原为Pd(0)。傅里叶变换红外光谱(FT-IR)、能谱分析(EDS)、X射线衍射(XRD)、热重分析(TGA)、透射电子显微镜(TEM)和扫描电子显微镜(SEM)图像是证明催化剂合成成功的特征方法。SEM图像显示颗粒尺寸为25-50nm,TEM图像证实存在尺寸小于2nm的钯纳米颗粒。催化剂的EDS元素分析证明了Pd、Fe和Al原子的存在,以及属于杂环部分的C、O、N和Si原子。振动样品磁强计(VSM)分析表明,最终催化剂的铁尖晶石核由于其表面改性,磁性显著下降。TGA曲线表明Pd@Her-TCT-PDA含有20%的有机成分,这归因于锚定的杂环配体。最后,将Pd@Her-TCT-PDA与硼氢化钠一起用作催化体系,将芳香族化合物的硝基完全还原为相应的胺。可回收性测试表明,Pd@Her-TCT-PDA在第三次运行后催化活性下降较低,钯纳米颗粒的浸出可忽略不计。