席夫碱修饰的SBA-15介孔分子筛的制备及其催化靛红参与的反应研究

发布时间：2018-04-02 22:25

本文选题：SBA-15　切入点：席夫碱　出处：《新疆大学》2016年硕士论文

【摘要】：介孔分子筛是一类孔径在2~50nm范围的纳米结构材料,具有较大的比表面积、高度有序的孔道结构、厚孔壁以及高的水热稳定性等优点。其孔道表面含有大量的硅羟基,利用这些羟基可以将一些有机分子固载于孔径内,是催化剂的优良载体。其中SBA-15介孔分子筛具有均匀的管状孔道、孔容以及较大的孔径(4~30nm范围内可调)等特点,可以通过内表面硅羟基负载活性组分或引入活性分子,制成非均相催化剂,使其具有催化活性,从而在分子催化领域具有广泛的用途。席夫碱是具有C=N双键的一类有机化合物,此类化合物及其金属络合物在医学、催化、分析化学、腐蚀以及光致变色等领域展现出重要的应用价值。其中,在催化领域,席夫碱在有机反应中可以提供有效的活性位点,表现出良好的催化性能。然而,在后处理阶段,由于席夫碱类催化剂在催化过程中与反应混合液形成均相体系,席夫碱的分离变得十分困难。基于SBA-15结构特点以及优良的物理化学性质,通过负载席夫碱,不仅提高了催化性能,而且能够重复使用多次,解决了催化剂的难分离、难回收等难题。本文将苯接三唑席夫碱嫁接于介孔分子筛SBA-15上,制备成固载型非均相催化剂,对其进行结构表征,并对其在有机反应中的催化性能进行研究。本论文主要包括以下两部分内容:第一部分文献综述,介绍固载型介孔分子筛SBA-15催化剂的研究进展及其应用;对固载型非均相催化剂在Knoevenagel缩合以及三组分反应中的研究进展进行阐述。第二部分实验部分,主要包括以下几个方面的内容:1.制备苯接三唑席夫碱以及介孔分子筛SBA-15/席夫碱催化剂,并对其进行了FI-IR、XRD、TEM及SEM表征。2.苯接三唑席夫碱改性的介孔分子筛SBA-15在水相介质中催化靛红与丙二腈以及氰基乙酸乙酯的Knoevenagel缩合反应的研究。3.苯接三唑席夫碱改性的介孔分子筛SBA-15催化靛红与吡唑啉酮的Knoevenagel缩合反应的研究。4.苯接三唑席夫碱改性的介孔分子筛SBA-15在水相介质中催化靛红、丙二腈与活泼二羰基类化合物的一锅法三组分反应的研究。
[Abstract]:Mesoporous molecular sieve is a kind of nanostructured materials with pore size in the range of 2~50nm. It has the advantages of large specific surface area, highly ordered pore structure, thick pore wall and high hydrothermal stability.There are a lot of silicon hydroxyl groups on the pore surface, which can be used to immobilize some organic molecules in the pore size, which is an excellent support for the catalyst.Among them, SBA-15 mesoporous molecular sieves have the characteristics of uniform tubular channels, pore volume and adjustable pore size in the range of 410nm. The heterogeneous catalysts can be prepared by loading active components on the inner surface of silica hydroxyl groups or introducing active molecules into the mesoporous molecular sieves.It has a wide range of applications in the field of molecular catalysis because of its catalytic activity.Schiff base is a class of organic compounds with Con N double bond. These compounds and their metal complexes have shown important application value in medicine, catalysis, analytical chemistry, corrosion and photochromic.In the field of catalysis, Schiff base can provide effective active sites in organic reactions and show good catalytic performance.However, in the post-treatment stage, the separation of Schiff base becomes very difficult because of the homogeneous system of Schiff base catalyst and reaction mixture in the catalytic process.Based on the structural characteristics of SBA-15 and its excellent physical and chemical properties, the supported Schiff base not only improves the catalytic performance, but also can be reused for many times, thus solving the difficult problems of separation and recovery of the catalyst.In this paper, the immobilized heterogeneous catalyst was prepared by grafting benzene with triazole Schiff base onto mesoporous molecular sieve SBA-15, and its structure was characterized, and its catalytic performance in organic reaction was studied.This paper mainly includes the following two parts: the first part is a review of the literature review, introduce the research progress and application of the immobilized mesoporous molecular sieve SBA-15 catalyst;The research progress of immobilized heterogeneous catalysts in Knoevenagel condensation and three component reactions was reviewed.The second part of the experiment, mainly includes the following aspects of the content: 1.Triazole Schiff base and mesoporous molecular sieve SBA-15/ Schiff base catalyst were prepared and characterized by TEM and SEM.Studies on the Knoevenagel condensation of indigo with malonitrile and ethyl cyanoacetate catalyzed by mesoporous molecular sieve SBA-15 modified by benzene triazole Schiff base in aqueous medium.Studies on the Knoevenagel condensation of indigo with pyrazolone catalyzed by mesoporous molecular sieve SBA-15 modified by benzene triazole Schiff base.One-pot reaction of indirubin, malonitrile and active dicarbonyl compounds catalyzed by mesoporous molecular sieve SBA-15 modified by benzene triazole Schiff base in aqueous medium was studied.
【学位授予单位】：新疆大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O643.36

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