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α-酮戊二酸超分子復(fù)合物的合成、結(jié)構(gòu)及性質(zhì)研究

發(fā)布時(shí)間:2018-01-19 05:22

  本文關(guān)鍵詞: 超分子復(fù)合物 α-酮戊二酸 原位分解 催化 抑菌 出處:《南昌大學(xué)》2015年碩士論文 論文類(lèi)型:學(xué)位論文


【摘要】:利用配位鍵和氫鍵、π···π作用等超分子作用構(gòu)筑的超分子復(fù)合物,不僅具有新穎的拓?fù)浣Y(jié)構(gòu),而且在氣體存儲(chǔ),氣體分離、發(fā)光、催化、生物活性等領(lǐng)域有潛在的應(yīng)用價(jià)值,因而新型超分子復(fù)合物的合成與性質(zhì)研究成為當(dāng)前關(guān)注的熱點(diǎn)。在超分子復(fù)合物的設(shè)計(jì)合成中,有機(jī)配體在構(gòu)筑超分子網(wǎng)絡(luò)結(jié)構(gòu)中起到?jīng)Q定性的作用。柔性配體具有更靈活的幾何構(gòu)型,更容易合成出結(jié)構(gòu)新穎和性質(zhì)特別的新型超分子復(fù)合物。本論文采用多齒柔性配體α-酮戊二酸合成了11個(gè)新的超分子復(fù)合物,利用單晶X-射線(xiàn)衍射、元素分析、IR、TGA和PXRD對(duì)其進(jìn)行表征了物化表征及性質(zhì)研究。1.用α-酮戊二酸與咪唑及其衍生物,在溶劑熱條件下,得到了10個(gè)超分子復(fù)合物。這10個(gè)化合物的自組裝過(guò)程中涉及典型的分子間氫鍵及其他非共價(jià)鍵的相互作用力,并且通過(guò)這些非共價(jià)鍵的相互作用,使得這10個(gè)化合物形成3D超分子結(jié)構(gòu)。結(jié)果表明,通過(guò)α-酮戊二酸和咪唑及其衍生物間的離子的或者中性的氫鍵O-H···N和氫鍵O-H···O能夠形成有機(jī)鹽和共晶。其中化合物1-7和10是有機(jī)鹽,而化合物8和9是共晶。將化合物2、3、5作為抑菌劑在濃度為25 mg/mL時(shí),對(duì)大腸桿菌有明顯的抑菌效果,而對(duì)金黃葡萄球菌則沒(méi)有。2.在溶劑熱條件下,利用α-酮戊二酸和2,2’-聯(lián)吡啶與乙酸銅原位合成了化合物11。晶體結(jié)構(gòu)測(cè)定表明,化合物11的配體為草酸和2,2’-bpy,α-酮戊二酸原位分解為草酸和丙二酸。通過(guò)分子間氫鍵和π···π作用形成三維超分子網(wǎng)絡(luò)結(jié)構(gòu)。考察了化合物11催化苯乙烯環(huán)氧化的催化性能。結(jié)果表明:在80°C,6 h時(shí),苯乙烯轉(zhuǎn)化率為47.2%,環(huán)氧苯乙烷的選擇性達(dá)到43.6%。此外,催化劑能連續(xù)使用2次而活性沒(méi)有明顯下降。
[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 偽 -ketoglutaric acid and single crystal X-ray diffraction. The physicochemical characterization and properties of the 偽 -ketoglutaric acid, imidazole and its derivatives were studied by elemental analysis, IR, TGA and PXRD. 1. Under solvothermal conditions, 偽 -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 偽 -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 偽 -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. 偽 -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 擄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.
【學(xué)位授予單位】:南昌大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2015
【分類(lèi)號(hào)】:O641.3;TB33

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