空心双壳型MOFs微球负载钯纳米粒子结构的设计、合成及其催化加氢研究

发布时间：2018-10-17 14:15

【摘要】：金属纳米粒子@金属有机骨架化合物(MNPs@MOFs)复合材料因其结构和功能的多样性而被广泛应用于催化、传感、气体吸附与分离等领域,并时常表现出优异于单一MOFs或者MNPs的性质。到目前为止,已经有越来越多的MNPs@MOFs结构被设计、合成出来。按照其MNPs在MOFs内的粒径大小、所处位置、合成方法以及整体形态来归纳,其主要分为“分散型”、“Core-shell”、“Yolk-shell”以及“Reverse bumpy ball”四种结构。结构的多样性往往可能导致性能或者应用价值的多样性。因此本文的主要内容是在总结前人经验的基础上,设计了一种新型的“空心双壳型”MOFs负载金属纳米粒子的MNPs@MOFs结构(Void@MOF/MNPs@MOF)。并成功制备了两例这种结构:Void@HKUST-1/Pd@ZIF-8型以及Void@ZIF-8/Pd@ZIF-8型,并将其应用于液相烯烃加氢反应。研究生期间的主要工作分为以下两个部分:第一部分:以磺化聚苯乙烯球为模板,参考文献,在其表面生长HKUST-1晶体,并将其用于作为内壳层来负载金属Pd纳米粒子,然后在负载Pd纳米粒子的HKUST-1壳层上,继续生长一层具有特殊孔道的ZIF-8晶体,最后除去模板SPS,得到带有空腔结构的Void@HKUST-1/Pd@ZIF-8微球。并将其用于催化液相选择性烯烃加氢反应。第二部分:延续第一部分的合成思路上,将合成相对费时的HKUST-1内壳层晶体成功替换为合成更为简便、稳定且和外壳层同晶型的ZIF-8晶体,最终得到Void@ZIF-8/Pd@ZIF-8微球,并将其用于催化苯乙烯加氢反应。
[Abstract]:Metal nanoparticles @ organometallic skeleton compound (MNPs@MOFs) composites have been widely used in catalysis, sensing, gas adsorption and separation due to their diversity of structure and function, and have been shown to be superior to single MOFs or MNPs. Up to now, more and more MNPs@MOFs structures have been designed and synthesized. According to the particle size, position, synthesis method and overall morphology of MNPs in MOFs, it can be divided into four types: "disperse type", "Core-shell", "Yolk-shell" and "Reverse bumpy ball". Structural diversity can often lead to diversity in performance or application value. Therefore, the main content of this paper is to design a new "hollow double shell" MOFs supported metal nanoparticles MNPs@MOFs structure (Void@MOF/MNPs@MOF) based on the previous experience. Two cases of this structure, Void@HKUST-1/Pd@ZIF-8 type and Void@ZIF-8/Pd@ZIF-8 type, were successfully prepared and applied to the hydrogenation of olefins in liquid phase. The main work of the graduate school was divided into the following two parts: the first part: HKUST-1 crystals were grown on the surface of sulfonated polystyrene spheres as template, and used as inner shell to load metal Pd nanoparticles. Then, a layer of ZIF-8 crystals with special pores was grown on the HKUST-1 shell loaded with Pd nanoparticles. Finally, Void@HKUST-1/Pd@ZIF-8 microspheres with cavity structure were obtained by removing template SPS,. It was used to catalyze liquid phase selective hydrogenation of olefins. The second part: continuation of the first part of the synthesis ideas, the synthesis of relatively time-consuming HKUST-1 inner shell crystal was successfully replaced with the synthesis of more convenient, stable and shell homocrystalline ZIF-8 crystal, and finally Void@ZIF-8/Pd@ZIF-8 microspheres. It was used to catalyze the hydrogenation of styrene.
【学位授予单位】：南昌大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB383.1;O643.36

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