本文選題：氧化吡啶 + 異相催化　； 參考：《山東師范大學》2017年碩士論文

【摘要】：配位聚合物的合成與性質研究是目前自組裝化學領域的研究熱點。超分子自組裝是分子通過分子間相互作用自行聚集,形成有序結構的聚集體現(xiàn)象,它往往表現(xiàn)出單個分子或低級分子聚集體所不具有的特性與功能。在本文中,我們設計合成了一系列氧化吡啶配體、苯并咪唑配體,并將其與過渡金屬進行自組裝,都得到了13例結構新穎,性質優(yōu)良的配位聚合物,利用粉末衍射、X-射線單晶衍射、紅外及熱重進行表征,并對其中具有代表性的配位聚合物進行了催化性質的研究。Ⅰ.利用本研究組內原有的兩例以吡啶為端基的氧化吡啶橋連有機配體,將其與過渡金屬進行自組裝,得到了5例結構新穎的配位聚合物。其中有4例配位聚合物中氧化吡啶集團上的氧原子沒有與金屬發(fā)生配位,因此利用氧化吡啶Lewis堿的性質來催化Knoevenagel縮合反應。作為異相催化劑,其可被重復利用5次,有著較高的催化效率和選擇性。Ⅱ將羧酸基團引入到氧化吡啶類有機配體中,在溶劑熱的條件下,與過渡金屬進行自組裝,得到了4例結構新穎且穩(wěn)定的配位聚合物,將參與配位的溶劑DMF分子與其他功能化的小分子交換,期待其用于氨基酸的識別。Ⅲ設計合成一系列苯并咪唑類的有機配體,與過渡金屬自組裝之后,得到了4例結構新穎的配位聚合物。在自組裝的過程中,配體發(fā)生了碳碳鍵的斷裂,并證明碳碳鍵斷裂之后的產物。
[Abstract]:The synthesis and properties of coordination polymers are the focus in the field of self-assembly chemistry. Supramolecular self-assembly is a kind of aggregation phenomenon in which molecules gather by themselves through intermolecular interaction to form an ordered structure. It often shows the characteristics and functions that a single molecule or a low molecular aggregate does not have. In this paper, a series of pyridine oxide ligands and benzimidazole ligands were designed and synthesized, which were self-assembled with transition metals. X-ray single crystal diffraction (XRD), infrared spectroscopy (IR) and thermogravimetry (TGA) were used to characterize the coordination polymers, and their catalytic properties were studied. Two pyridine oxide bridged organic ligands with pyridine as terminal group were used in this study to self-assemble with transition metals, and five novel coordination polymers were obtained. In four of the coordination polymers, the oxygen atoms on the pyridine oxide group did not coordinate with the metal, so the properties of the pyridine oxide Lewis base were used to catalyze the condensation of Knoevenagel. As a heterogeneous catalyst, it can be reused for 5 times, and has high catalytic efficiency and selectivity. II the carboxylic acid group is introduced into the organic ligand of pyridine oxide and self-assembled with transition metal under solvothermal conditions. Four novel and stable coordination polymers were obtained. The solvent DMF molecules involved in the coordination were exchanged with other functionalized small molecules, which were expected to be used in the recognition of amino acids. III. A series of benzimidazole organic ligands were designed and synthesized. After self-assembly with transition metal, four novel coordination polymers were obtained. In the process of self-assembly, the ligand had the rupture of carbon and carbon bond, and it was proved that the product after the breaking of carbon and carbon bond.
【學位授予單位】：山東師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O641.4
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本文編號：1893728