苯并咪唑功能化COFs材料的构建及催化性能

发布时间：2018-05-05 05:33

本文选题：共价有机框架材料 + 苯并咪唑　；参考：《兰州大学》2015年硕士论文

【摘要】：共价有机框架材料(Covalent Organic Frameworks, COFs)是一种晶型的、纯有机的、共价键连接的多孔材料。由于具有较低的密度、较高的稳定性、较大的比表面积以及易于功能化等特点,COFs材料在气体吸附/存储、光电和催化等领域均具有重要的应用价值。但是,目前有关功能化COFs材料报道还比较少。我们以苯并咪唑为功能化前体,设计合成了苯并咪唑及其衍生的氮杂卡宾功能化的COFs材料,并实现了它们在多相催化中的应用。本论文的研究工作主要分为两部分：(1)以苯并咪唑为前体,合成了两种亚胺键连接的苯并咪唑功能化COFs材料,分别为COF-LZU30和COF-LZU31。COF-LZU30和COF-LZU31均具有规整的2D孔道结构和较大的比表面积,且能够在室温的条件下催化Knoevenagel缩合反应。由于咪唑催化活性位点在COF孔道内均匀的分布,COF-LZU31在非质子性溶剂中催化Knoevenagel缩合反应的活性高于其对应的均相体系。(2)在苯并咪唑功能化COFs材料的基础上,我们尝试了通过"bottom-up"和‘'post-synthesis"策略来构建氮杂卡宾功能化的COFs材料,并对'post-synthesis"策略对材料稳定性的影响进行了探究。同时,我们也尝试了氮杂金属卡宾功能化COFs材料的合成。
[Abstract]:Covalent Organic frameworks (COFs) is a crystalline, pure organic, covalently bonded porous material. Because of its low density, high stability, large specific surface area and easy functionalization, COFs have important application value in gas adsorption / storage, photoelectricity and catalysis. However, there are few reports about functionalized COFs materials. Benzimidazole and its derivatives of azacarbene functionalized COFs materials were designed and synthesized with benzimidazole as the functionalized precursor and their applications in heterogeneous catalysis were realized. In this paper, two kinds of benzimidazole functional COFs materials were synthesized by using benzimidazole as precursor. The results show that COF-LZU30, COF-LZU31.COF-LZU30 and COF-LZU31 have regular 2D pore structure and large specific surface area, respectively. It can catalyze the condensation of Knoevenagel at room temperature. Because the catalytic activity sites of imidazole are uniformly distributed in COF channels, the catalytic activity of COF-LZU31 for Knoevenagel condensation in non-proton solvent is higher than that of its homogenous system. (2) on the basis of benzimidazole functionalized COFs materials, the catalytic activity of COF-LZU31 is higher than that of its homogenous system. We try to construct azacarbin functionalized COFs materials by "bottom-up" and post-synthesis strategies, and explore the effect of post-synthesis strategy on the stability of COFs materials. At the same time, we have also tried to synthesize the COFs materials of carbene functionalization.
【学位授予单位】：兰州大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TB383.4

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