α-酮戊二酸超分子复合物的合成、结构及性质研究

发布时间：2018-01-19 05:22

本文关键词： 超分子复合物 α-酮戊二酸原位分解催化抑菌　出处：《南昌大学》2015年硕士论文　论文类型：学位论文

【摘要】：利用配位键和氢键、π···π作用等超分子作用构筑的超分子复合物,不仅具有新颖的拓扑结构,而且在气体存储,气体分离、发光、催化、生物活性等领域有潜在的应用价值,因而新型超分子复合物的合成与性质研究成为当前关注的热点。在超分子复合物的设计合成中,有机配体在构筑超分子网络结构中起到决定性的作用。柔性配体具有更灵活的几何构型,更容易合成出结构新颖和性质特别的新型超分子复合物。本论文采用多齿柔性配体α-酮戊二酸合成了11个新的超分子复合物,利用单晶X-射线衍射、元素分析、IR、TGA和PXRD对其进行表征了物化表征及性质研究。1.用α-酮戊二酸与咪唑及其衍生物,在溶剂热条件下,得到了10个超分子复合物。这10个化合物的自组装过程中涉及典型的分子间氢键及其他非共价键的相互作用力,并且通过这些非共价键的相互作用,使得这10个化合物形成3D超分子结构。结果表明,通过α-酮戊二酸和咪唑及其衍生物间的离子的或者中性的氢键O-H···N和氢键O-H···O能够形成有机盐和共晶。其中化合物1-7和10是有机盐,而化合物8和9是共晶。将化合物2、3、5作为抑菌剂在浓度为25 mg/mL时,对大肠杆菌有明显的抑菌效果,而对金黄葡萄球菌则没有。2.在溶剂热条件下,利用α-酮戊二酸和2,2’-联吡啶与乙酸铜原位合成了化合物11。晶体结构测定表明,化合物11的配体为草酸和2,2’-bpy,α-酮戊二酸原位分解为草酸和丙二酸。通过分子间氢键和π···π作用形成三维超分子网络结构。考察了化合物11催化苯乙烯环氧化的催化性能。结果表明:在80°C,6 h时,苯乙烯转化率为47.2%,环氧苯乙烷的选择性达到43.6%。此外,催化剂能连续使用2次而活性没有明显下降。
[Abstract]:The supramolecular complexes constructed by supramolecular interaction, such as coordination bond and hydrogen bond, 蟺路路蟺, not only have novel topological structure, but also are used in gas storage, gas separation, luminescence and catalysis. Biological activity and other fields have potential application value, so the synthesis and properties of new supramolecular complexes have become the focus of attention. In the design and synthesis of supramolecular complexes. Organic ligands play a decisive role in building supramolecular networks. Flexible ligands have a more flexible geometric configuration. It is easier to synthesize new supramolecular complexes with novel structure and special properties. In this paper, 11 new supramolecular complexes were synthesized by using polydentate flexible ligand 伪 -ketoglutaric acid and single crystal X-ray diffraction. The physicochemical characterization and properties of the 伪 -ketoglutaric acid, imidazole and its derivatives were studied by elemental analysis, IR, TGA and PXRD. 1. Under solvothermal conditions, 伪 -ketoglutaric acid, imidazole and its derivatives were used. Ten supramolecular complexes have been obtained which involve typical intermolecular hydrogen bonds and other noncovalent bond interactions in the self-assembly process of these 10 compounds and through the interaction of these non-covalent bonds. The results show that the 10 compounds form 3D supramolecular structure. Organic salts and eutectics can be formed by the ionic or neutral hydrogen bonds O-H 路路N and O-H 路O between 伪 -ketoglutaric acid and imidazole and their derivatives. Compounds 1-7 and 10 are organic. Salt. Compounds 8 and 9 were eutectic. When the concentration of compound 2C 3N 5 was 25 mg/mL, it had obvious bacteriostasis effect on Escherichia coli. However, for Staphylococcus aureus, compound 11 was synthesized in situ using 伪 -ketoglutaric acid, 2-dipyridyl and copper acetate under solvothermal conditions. The crystal structure of the compound was determined. The ligands of compound 11 are oxalic acid and 2o 2n-BPY. 伪 -ketoglutaric acid was decomposed into oxalic acid and malonic acid in situ. The three-dimensional supramolecular network structure was formed by intermolecular hydrogen bond and 蟺路路蟺. The catalytic performance of compound 11 for styrene epoxidation was investigated. Clear:. At 80 掳C. At 6 h, the conversion of styrene was 47.2 and the selectivity of epoxy-phenylethane was 43.6. In addition, the catalyst could be used continuously for two times without obvious decrease in activity.
【学位授予单位】：南昌大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：O641.3;TB33

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