【摘要】：與傳統(tǒng)雙水相相比,離子液體雙水相具有分相快、粘度低、幾乎無乳化現(xiàn)象等優(yōu)點(diǎn),在萃取分離領(lǐng)域得到了廣泛的關(guān)注。隨著對(duì)離子液體研究的逐漸深入,人們發(fā)現(xiàn),在傳統(tǒng)的離子液體-無機(jī)鹽雙水相體系中,咪唑類/吡啶類離子液體的生物/環(huán)境毒性和高濃度無機(jī)鹽廢水的產(chǎn)生,在一定程度上限制了它們的可持續(xù)應(yīng)用。解決這些問題的關(guān)鍵是發(fā)展環(huán)境友好的離子液體雙水相體系。可生物降解的膽堿離子液體可以參與形成環(huán)境友好的離子液體雙水相,但是膽堿類離子液體的結(jié)構(gòu)相對(duì)簡(jiǎn)單,能夠與它們形成雙水相的成相物質(zhì)很少。作為國家自然科學(xué)基金資助課題(No.21133009)研究工作的一部分本文從環(huán)境友好的乙二醇衍生物出發(fā),設(shè)計(jì)、合成了一系列具有膽堿結(jié)構(gòu)的離子液體。在此基礎(chǔ)上,系統(tǒng)研究了這些離子液體與熱響應(yīng)聚合物EOPO形成雙水相的相平衡性質(zhì)及其對(duì)綠原酸、咖啡酸等植物化學(xué)品的選擇性分離,主要研究內(nèi)容包括:1.設(shè)計(jì)、合成了24種功能化膽堿離子液體,使用核磁共振光譜(~1H NMR,13C NMR)、差示掃描量熱(DSC)和熱重分析(TGA)等技術(shù)對(duì)這些離子液體進(jìn)行表征。結(jié)果表明,這些離子液體具有優(yōu)良的低溫性能及良好的熱穩(wěn)定性,屬于室溫離子液體的范疇。2.測(cè)定了本文所合成的功能化膽堿離子液體與EOPO 1900,EOPO2000,EOPO2700和EOPO5800等熱響應(yīng)聚合物形成雙水相體系的液-液平衡數(shù)據(jù),構(gòu)建了功能化膽堿離子液體-聚合物雙水相體系的液-液平衡相圖,系統(tǒng)研究了離子液體和聚合物的結(jié)構(gòu),體系的溫度等因素對(duì)離子液體雙水相相平衡的影響,深入分析了這類雙水相體系的成相規(guī)律。3.研究了綠原酸和咖啡酸在功能化膽堿離子液體-聚合物雙水相體系中的分配行為,系統(tǒng)討論了雙水相組成、綠原酸和咖啡酸的分子結(jié)構(gòu)等因素對(duì)它們分配性能的影響,建立了基于離子液體-聚合物雙水相體系的綠原酸和咖啡酸綠色分離方法。研究結(jié)果表明,在優(yōu)化的條件下,通過一步萃取,這類雙水相體系對(duì)綠原酸和咖啡酸的萃取率最高可分別達(dá)到97.0%和96.7%。4.研究了功能化膽堿離子液體-聚合物雙水相體系對(duì)綠原酸和咖啡因的選擇性分離性能,分析了相組分的濃度、聚合物的結(jié)構(gòu)、體系的溫度等因素對(duì)選擇性分離性能的影響,提出了一種基于環(huán)境友好離子液體雙水相體系的綠原酸和咖啡因的選擇性分離方法。在優(yōu)化條件下,通過一步萃取,綠原酸和咖啡因在雙水相體系中的選擇性分離系數(shù)最高可以達(dá)到195。
[Abstract]:Compared with traditional aqueous two-phase, ionic liquid aqueous two-phase has many advantages, such as fast phase separation, low viscosity, almost no emulsification and so on, and has been widely concerned in the field of extraction and separation. With the further study of ionic liquids, it has been found that in the traditional ionic liquid-inorganic salt aqueous two-phase system, the biological / environmental toxicity of imidazole / pyridine ionic liquids and the production of high concentration inorganic salt wastewater are observed. To some extent, it limits their sustainable application. The key to solve these problems is to develop environmental friendly ionic liquid aqueous two-phase system. Biodegradable choline ionic liquids can participate in the formation of environment-friendly aqueous ionic liquids, but the structure of choline ionic liquids is relatively simple. As part of the research work supported by National Natural Science Foundation (No.21133009), a series of ionic liquids with choline structure were designed and synthesized from the environmentally friendly ethylene glycol derivatives. On this basis, the phase equilibrium properties of these ionic liquids and thermally responsive polymer EOPO to form aqueous two-phase and their selective separation for plant chemicals such as Lv Yuan acid and caffeic acid were systematically studied. The main research contents include: 1. Twenty-four functional choline ionic liquids were designed and synthesized and characterized by 1H NMR-13C NMR), differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA). The results show that these ionic liquids have excellent low temperature properties and good thermal stability, which belong to the category of room temperature ionic liquids. The liquid-liquid equilibrium data of the functionalized choline ionic liquid synthesized in this paper and the thermo-responsive polymers such as EOPO 1900 and EOPO2700 and EOPO5800 were measured, and the liquid-liquid equilibrium diagram of the functionalized choline ion liquid-polymer aqueous two-phase system was constructed. The effects of the structure of ionic liquid and polymer and the temperature of the system on the phase equilibrium of aqueous two-phase ionic liquid were systematically studied. The phase formation law of this kind of aqueous two-phase system was analyzed in depth. The partition behavior of Lv Yuan acid and caffeic acid in functionalized choline ionic liquid-polymer aqueous two-phase system was studied. The effects of the composition of aqueous two-phase and the molecular structure of Lv Yuan acid and caffeic acid on their partition properties were discussed systematically. A green separation method for Lv Yuan acid and caffeic acid was established based on ionic liquid-polymer aqueous two-phase system. The results show that under the optimized conditions, the extraction rates of Lv Yuan acid and caffeic acid can be up to 97.0% and 96.70..4 respectively by one-step extraction of this two-phase aqueous system. The selective separation of Lv Yuan acid and caffeine by functionalized choline ionic liquid-polymer aqueous two-phase system was studied. The effects of phase concentration, polymer structure and system temperature on the selective separation performance were analyzed. A selective separation method of Lv Yuan acid and caffeine based on environmental friendly ionic liquid aqueous two-phase system was proposed. Under the optimized conditions, the highest selective separation coefficients of Lv Yuan acid and caffeine in aqueous two-phase system can be obtained by one-step extraction.
【學(xué)位授予單位】：河南師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O658.2

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本文編號(hào)：2196338