丁二酰胺基功能性离子液的合成表征以及对铀酰、钍、铕的萃取行为研究

发布时间：2018-08-08 16:50

【摘要】：随着世界各国的经济快速发展,同时也带来了很多环境、能源等严重性社会问题,为了解决电力能源的需求问题,当代核工业正在快速发展,原料铀的处理工艺以及在核电后期的高放废液中的铀处理工艺都是引起广泛专注的,解决此类问题才能使核能走向更加宽广的应用前景,才能在未来更加长久地使用下去。本文采用新型的功能性离子液体进行萃取处理,作为一种新型的萃取手段,成为了多方关注的焦点,功能性离子液体用于萃取研究,主要发挥了离子液体低挥发性、低粘度、无毒无污染、可重复使用的优点,同时又具备特殊的萃取功能基团,实现萃取分离。本文合成并且表征了3-双(N,N-R基氨基甲酰基)-1-R’基咪唑NTf2功能性离子液萃取剂。本文涉及到的几种萃取剂合成原料简单易得,合成方法可以适用于大量合成,具有较好的工业使用前景。本文共合成了7种不同取代基的丁二酰胺类功能性离子液,并且通过有机合成过程中经常使用的高分辨质谱、红外光谱、核磁共振氢谱、碳谱对产物的结构进行了相应的表征确认。本文同时探究了不同功能性离子液体在常规有机溶剂作稀释剂,离子液作稀释剂,不使用稀释剂三种情况下的萃取情况,在不同酸度,不同浓度以及不同振荡时间下的萃取情况,反萃和重复使用。实验结果证明:首先合成了七种新型功能性离子液体,其中合成的丁二酰胺基离子液3-双(N,N-丁基氨基甲酰基)-1丁基咪唑双三氟甲磺酰功能性离子液在铀酰的萃取行为研究中表现出最好的效果,并且对钍和铕的萃取性能很差,有望应用于镧锕分离研究,其在没有稀释剂参与的情况下功能性离子液的萃取效果更好;在不同氢离子浓度的条件下对铀酰的萃取效果,表现出的趋势是当氢离子浓度越大,铀酰离子更加容易进行萃取;一定范围内延长振荡时间,功能性离子液体的萃取效果会增强,在70分钟时萃取达到平衡;功能性离子液阴离子不交换的基础上依旧具有较好的萃取性能;功能性离子液可多次重复利用。
[Abstract]:With the rapid economic development of various countries in the world, it has also brought many serious social problems such as environment, energy and so on. In order to solve the problem of the demand for power energy, the contemporary nuclear industry is developing rapidly. The treatment process of raw uranium and the uranium treatment process in the high-level radioactive waste liquid in the late stage of nuclear power have caused extensive attention. Only by solving this kind of problems can nuclear energy be more widely used and can it be used for a longer time in the future. In this paper, a new type of functional ionic liquid is used for extraction, as a new method of extraction, it has become the focus of attention. Functional ionic liquid is used in extraction research, which mainly plays the role of low volatility and low viscosity of ionic liquid. It has the advantages of no toxicity and no pollution, can be reused, and has special extraction functional groups to realize extraction separation. The functional ionic liquid extractant of 3-bis (N-R carbamoyl) -1-R' imidazole (NTf2) was synthesized and characterized. The synthetic raw materials of several extractants involved in this paper are simple and easy to obtain, and the synthetic methods can be used in a large number of synthesis, and have a good prospect of industrial use. In this paper, seven kinds of succinamide functional ionic liquids with different substituents have been synthesized, and the high resolution mass spectrometry, infrared spectrum, nuclear magnetic resonance hydrogen spectrum, which are often used in the organic synthesis process, have been used. The structure of the product was confirmed by carbon spectrum. At the same time, the extraction conditions of different functional ionic liquids in conventional organic solvents, ionic liquids as diluents, no diluents used, and different acidity were investigated. Extraction under different concentration and different oscillation time, stripping and reuse. The experimental results show that seven new functional ionic liquids have been synthesized. The 3- bis (N- N- Ding Ji carbamate)-1 Ding Ji imidazole bis-trifluoromethane sulfonyl functional ionic liquid synthesized from succinamide ionic liquid showed the best effect in the study of the extraction behavior of uranyl, and the extraction performance of thorium and europium was very poor. It is expected to be applied to the separation of lanthanides, whose extraction effect is better than that of functional ionic liquid without diluent, and the tendency of extraction of uranyl at different concentrations of hydrogen ions is that the higher the concentration of hydrogen ion, It is easier to extract uranyl ions, and if the oscillation time is prolonged, the extraction effect of functional ionic liquids will be enhanced, and the extraction equilibrium will be reached at 70 minutes. On the basis of functional ionic liquid anion exchange, it still has good extraction performance, and functional ionic liquid can be reused many times.
【学位授予单位】：兰州大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O658.2;O645.1

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