功能化离子液体催化合成环状碳酸酯的研究

发布时间：2018-03-11 06:19

本文选题：CO_2转化　切入点：环状碳酸酯　出处：《渤海大学》2017年硕士论文　论文类型：学位论文

【摘要】：二氧化碳与环氧化合物反应合成环状碳酸酯是化学固定转化CO_2的一个重要反应,是实现碳减排的一个重要途径。利用化学方法将CO_2作为碳资源转化为大宗化工原料,是目前二氧化碳规模利用领域的希望和关注方向之一,而开发绿色无毒、易分离的环加成反应催化剂是当前研究的重要课题。因此本论文设计并合成不同尺寸的聚合离子液体、甲基丙烯酸氨基酯类离子液体催化转化CO_2生成环状碳酸酯,并分析了反应条件对催化剂活性及选择性的影响。合成了聚多巴胺(PDA)功能化的聚合离子液体催化剂,并考察其在CO_2与环氧化合物合成环状碳酸酯中的反应性能。结果表明,溴乙烷改性的170nm聚多巴胺聚合物(170nmPDAEBr)因分子中含有的多羟基和卤素离子协同强化诱导环氧化合物开环,使其具有良好的催化效果。在无助剂及温和条件下(120 oC,3 MPa)反应3 h,环氧丙烷(PO)的转化率达到99%,碳酸丙烯酯(PC)的选择性高于99%。合成了四种含有甲基丙烯酸氨基酯类离子液体,并在无助剂的条件下考察了样品对CO_2与环氧化合物合成环状碳酸酯反应的催化性能。其中用溴乙醇功能化甲基丙烯酸二甲氨乙酯([DMAEMA-Et][Br])为催化剂活性最好,在温和条件(120 oC,2 MPa)反应2 h,环氧丙烷转化率可高达99%,碳酸丙烯酯选择性也高于99%。
[Abstract]:The synthesis of cyclic carbonate by reaction of carbon dioxide with epoxy compound is an important reaction of chemical immobilization and conversion of CO_2 and an important way of carbon abatement. The chemical method is used to convert CO_2 as carbon resource to bulk chemical raw material. It is one of the promising and concerned fields in the field of scale utilization of carbon dioxide, and the development of green, non-toxic and easily separated cycloaddition reaction catalysts is an important research topic at present. Therefore, different sizes of polymeric ionic liquids are designed and synthesized in this paper. Amino methacrylate ionic liquid was used to catalyze the conversion of CO_2 to cyclic carbonate, and the effects of reaction conditions on the activity and selectivity of the catalyst were analyzed. The properties of the reaction in the synthesis of cyclic carbonates from CO_2 and epoxy compounds were investigated. The results showed that the polyhydroxyl groups and halogen ions in the modified polydopamine polymer (PDAEBr), modified by bromoethane, induced the ring opening of epoxide compounds by synergistic strengthening of polyhydroxyl groups and halogen ions. The conversion of propylene oxide (PO) was 99% and the selectivity of propylene carbonate (PC) was higher than 99%. Four kinds of ionic liquids containing amino methacrylate were synthesized. The catalytic properties of the samples for the synthesis of cyclic carbonate from CO_2 and epoxy compounds were investigated without any additives. The best catalytic activity was [DMAEMA-Et] [Br], in which bromoethanol was used as the functional catalyst for the synthesis of cyclic carbonate. The propylene oxide conversion was up to 99% and the selectivity of propylene carbonate was higher than that of 99% propene carbonate under mild conditions (120oC ~ (2) MPa) for 2 h.
【学位授予单位】：渤海大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O624.5

【相似文献】