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

【摘要】：配位聚合物的合成與性質(zhì)研究是目前自組裝化學(xué)領(lǐng)域的研究熱點(diǎn)。超分子自組裝是分子通過(guò)分子間相互作用自行聚集,形成有序結(jié)構(gòu)的聚集體現(xiàn)象,它往往表現(xiàn)出單個(gè)分子或低級(jí)分子聚集體所不具有的特性與功能。在本文中,我們?cè)O(shè)計(jì)合成了一系列氧化吡啶配體、苯并咪唑配體,并將其與過(guò)渡金屬進(jìn)行自組裝,都得到了13例結(jié)構(gòu)新穎,性質(zhì)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(jìn)行表征,并對(duì)其中具有代表性的配位聚合物進(jìn)行了催化性質(zhì)的研究。Ⅰ.利用本研究組內(nèi)原有的兩例以吡啶為端基的氧化吡啶橋連有機(jī)配體,將其與過(guò)渡金屬進(jìn)行自組裝,得到了5例結(jié)構(gòu)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(tuán)上的氧原子沒(méi)有與金屬發(fā)生配位,因此利用氧化吡啶Lewis堿的性質(zhì)來(lái)催化Knoevenagel縮合反應(yīng)。作為異相催化劑,其可被重復(fù)利用5次,有著較高的催化效率和選擇性。Ⅱ?qū)Ⅳ人峄鶊F(tuán)引入到氧化吡啶類(lèi)有機(jī)配體中,在溶劑熱的條件下,與過(guò)渡金屬進(jìn)行自組裝,得到了4例結(jié)構(gòu)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(shí)別。Ⅲ設(shè)計(jì)合成一系列苯并咪唑類(lèi)的有機(jī)配體,與過(guò)渡金屬自組裝之后,得到了4例結(jié)構(gòu)新穎的配位聚合物。在自組裝的過(guò)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(chǎn)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(xué)位授予單位】：山東師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：O641.4
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本文編號(hào)：1893728