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Preparation and characterization of Ni/mZSM-5 zeolite with a hierarchical pore structure by using KIT-6 as silica template: an efficient bi-functional catalyst for the reduction of nitro aromatic compounds

机译:以KIT-6为二氧化硅模板制备具有分级孔结构的Ni / mZSM-5沸石及其表征

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摘要

Ni/mZSM-5 and Ni/H-mZSM-5 were synthesized as hierarchical (micro/meso porous) ZSM-5 zeolites by an indirect template method for the first time. The resulting zeolite materials exhibited significantly enhanced diffusional properties in comparison to purely microporous zeolite materials. The structural and morphological characterization of the prepared catalysts was investigated using XRD, BET, atomic absorption spectroscopy, FT-IR, Al-27-MAS NMR, SEM, TEM, XPS and DRS-UV techniques. These hierarchical zeolites were used as acid-metal bi-functional heterogeneous catalysts for hydride transfer in the reduction of nitro aromatic compounds. In these reactions, NaBH4 was used as a reducing agent. Excellent yields at room temperature and very short reaction times in aqueous media conditions were obtained. Reusability experiments showed the excellent stability of Ni/mZSM-5 and Ni/H-mMZSM-5 and the catalysts could be reused 7 times without much loss of activity in reduction of nitro aromatic compounds. Surprisingly, the acid form of Ni/H-mZSM-5 showed much higher activity than that of Ni/mZSM-5. High yield, short reaction time, green solvent (water), room temperature, no by-product, the easy reusability of catalysts and the low amounts of catalyst required are some of the advantages of these catalysts.
机译:Ni / mZSM-5和Ni / H-mZSM-5首次通过间接模板法合成为分层(微孔/中孔)ZSM-5沸石。与纯微孔沸石材料相比,所得沸石材料表现出显着增强的扩散性能。使用XRD,BET,原子吸收光谱,FT-IR,Al-27-MAS NMR,SEM,TEM,XPS和DRS-UV技术研究了制备的催化剂的结构和形态表征。这些分级沸石被用作酸金属双官能多相催化剂,用于还原硝基芳族化合物中的氢化物转移。在这些反应中,将NaBH 4用作还原剂。在室温下获得了优异的产率,在水性介质条件下的反应时间非常短。可重复使用性实验表明,Ni / mZSM-5和Ni / H-mMZSM-5具有出色的稳定性,该催化剂可重复使用7次,而不会降低硝基芳族化合物的还原活性。令人惊讶的是,Ni / H-mZSM-5的酸形式显示出比Ni / mZSM-5更高的活性。高产率,短反应时间,绿色溶剂(水),室温,无副产物,催化剂易于重用和所需催化剂量低是这些催化剂的一些优点。

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