發(fā)布時(shí)間：2018-03-23 10:17

  本文選題：離子液體功能化　切入點(diǎn)：設(shè)計(jì)合成　出處：《西安工程大學(xué)》2015年碩士論文

【摘要】：功能化離子液體是完全由陰陽(yáng)離子組成的,在陰陽(yáng)離子中引入一個(gè)或多個(gè)官能團(tuán),使得其具有某種功能或特性的鹽類化合物。這種特定的分子結(jié)構(gòu)使得功能化離子液體具有特定功能、寬液態(tài)范圍、寬電化學(xué)窗口等獨(dú)特性質(zhì),其應(yīng)用領(lǐng)域涉及新型導(dǎo)電功能材料、有機(jī)合成、分離純化及生物催化等諸多領(lǐng)域。然而,離子液體分子的結(jié)構(gòu)解析、結(jié)構(gòu)與性質(zhì)之間的構(gòu)效關(guān)系等研究相對(duì)滯后,新型功能化離子液體的設(shè)計(jì)合成及選擇性應(yīng)用存在較大的難度。本論文首先從分子結(jié)構(gòu)設(shè)計(jì)的角度出發(fā),以吡啶、二乙烯吡啶、鹵代酯、鹵代酸和鹵代烷烴為反應(yīng)物,設(shè)計(jì)合成了多種吡啶類功能化離子液體,即含酯基的吡啶類功能化離子液體、含羧基的吡啶類功能化離子液體、聚吡啶類功能化離子液體單體及其聚合物,并系統(tǒng)研究了反應(yīng)溫度、反應(yīng)配比、反應(yīng)時(shí)間對(duì)吡啶類功能化離子液體合成過(guò)程的影響,確定其適宜反應(yīng)條件。其次,通過(guò)傅里葉紅外光譜技術(shù)以及核磁共振光譜技術(shù)等分析了功能化吡啶類離子液體的結(jié)構(gòu),并用單晶X射線衍射技術(shù),對(duì)[MEPy][PF6]的大單晶體結(jié)構(gòu)進(jìn)行解析,該化合物的空間群為P2(1)/n,晶型屬于單斜晶系,晶胞參數(shù)為a=14.30(2)nm,b=8.281(14)nm,c=29.48(5)nm,β=95.06o,Z=4,V=3.477(2)nm3,Dc=1.641 Mg/m3,μ=0.308 mm-1,F(000)=1676。進(jìn)一步對(duì)功能化吡啶類離子液體的導(dǎo)電性分析表明,含酯基和含羧基的功能化離子液體的電導(dǎo)率相對(duì)較大,聚離子液體的電導(dǎo)率相對(duì)較小,與單體相比較其電導(dǎo)率相差1個(gè)數(shù)量級(jí),且電導(dǎo)率導(dǎo)電行為符合Arrhenius方程。同時(shí)對(duì)其溶解性和熱穩(wěn)定性的研究表明,其極性接近于醇、酮,其中含酯基的吡啶類功能化離子液體的熱穩(wěn)定性相對(duì)較好。最后,將吡啶類功能化離子液體引入苯乙烯懸浮聚合體系成功制備了聚苯乙烯微球。研究表明,在體系中引入含酯基的離子液體時(shí),所制備的聚苯乙烯微球粒徑分布較為均勻,微球平均粒徑最小。同時(shí),吡啶類功能化離子液體在聚苯乙烯微球的成球過(guò)程中具有降低體系表面能,減弱微球間的團(tuán)聚等多重作用。通過(guò)對(duì)吡啶類離子液體的功能化研究,設(shè)計(jì)合成了含酯基的吡啶類功能化離子液體、含羧基的吡啶類功能化離子液體、聚吡啶類功能化離子液體單體及其聚合物,并將其首次引入苯乙烯聚合體系中制備了多孔結(jié)構(gòu)的聚合物微球,這將為多孔聚合物材料的制備提供一種新的思路。
[Abstract]:Functionalized ionic liquids are composed entirely of anions, in which one or more functional groups are introduced. A salt compound that has certain functions or properties. This particular molecular structure gives functionalized ionic liquids unique properties such as specific functions, wide liquid ranges, wide electrochemical windows, etc. Its applications include novel conductive functional materials, organic synthesis, separation and purification, biocatalysis and so on. However, the studies of structure resolution and structure-activity relationship between structure and properties of ionic liquids are relatively lagging behind. The design, synthesis and selective application of new functionalized ionic liquids are difficult. In this paper, pyridine, divinylpyridine, halogenated esters, halogenated acids and halogenated hydrocarbons are used as reactants from the point of view of molecular structure design. Several kinds of pyridine functionalized ionic liquids were designed and synthesized, including ester containing pyridine functionalized ionic liquids, carboxyl pyridine functional ionic liquids, polypyridine functionalized ionic liquids and their polymers. The effects of reaction temperature, reaction ratio and reaction time on the synthesis of pyridine functionalized ionic liquids were studied systematically. The structure of functionalized pyridine ionic liquids was analyzed by Fourier transform infrared spectroscopy (FTIR) and nuclear magnetic resonance spectroscopy (NMR). The large single crystal structure of [MEPy] [PF6] was analyzed by single crystal X-ray diffraction technique. The space group of the compound is P2N / 1 / n, and the crystal form belongs to monoclinic system. The cell parameters of the compound are as follows: a ~ (14.30) m ~ (-1) ~ (2) ~ (-) ~ (-) ~ (8) nmb ~ (1) C ~ (29) 485nm ~ (m), 尾 _ (95.06oC) ~ (3.4772nm) ~ (1.641)% Mgm ~ (3), 渭 ~ (0.308) m ~ (-1) ~ (-1) F ~ (000N) ~ (-1), and the conductivity of functionalized ionic liquids containing ester and carboxyl group is relatively large, the results show that the conductivity of functionalized ionic liquids containing ester and carboxyl group is relatively large. The results show that the ionic conductivity of functionalized ionic liquids containing ester group and carboxyl group is relatively large. The conductivity of polyionic liquids is relatively small, and the conductivity of polyionic liquids is 1 order of magnitude lower than that of monomers. The conductivity of polyionic liquids conforms to the Arrhenius equation. The solubility and thermal stability of polyionic liquids are similar to those of alcohols and ketones. The thermal stability of pyridine functionalized ionic liquids containing ester group was relatively good. Finally, polystyrene microspheres were successfully prepared by introducing pyridine functionalized ionic liquids into styrene suspension polymerization system. When the ester containing ionic liquid was introduced into the system, the particle size distribution of the prepared polystyrene microspheres was more uniform, and the average diameter of the microspheres was the smallest. Pyridine functionalized ionic liquids can reduce the surface energy of polystyrene microspheres, weaken the agglomeration of microspheres, etc. The functionalization of pyridine ionic liquids is studied. The functional ionic liquids containing ester group pyridine group, pyridine functional ionic liquid containing carboxyl group, polypyridine functional ionic liquid monomer and its polymer were designed and synthesized. The polymer microspheres with porous structure were prepared by introducing them into styrene polymerization system for the first time, which will provide a new way of thinking for the preparation of porous polymer materials.
【學(xué)位授予單位】：西安工程大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O645.1

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