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Alternative TitleSynthesis and CO2 Capture Study of Novel Dual Amino Functionalized Ionic Liquids
Thesis Advisor张锁江 ; 张香平
Degree Grantor中国科学院研究生院
Degree Discipline化学工程
Keyword离子液体   氨基功能化   co2捕集
Abstract二氧化碳(CO2)是最主要的温室气体之一,主要由燃烧煤炭、石油、天然气等化石燃料的使用所产生。大量的CO2气体进入大气中将会造成全球气候变暖,对生态环境构成巨大威胁。因此,二氧化碳的捕集分离成为新的研究热点之一。由于离子液体具有可忽略的蒸汽压、较高的热稳定性、较好的溶解CO2的能力,所以设计并合成能够高效捕集吸收CO2的新型氨基功能化离子液体对形成低能耗高效捕集分离技术具有重要意义。本论文的主要研究内容和取得的成果如下: 1. 设计并合成了两种新型的双氨基功能化离子液体,1,3-二(2′-氨基乙基)-2-甲基咪唑溴盐(DAIL-Br)和1,3-二(2′-氨基乙基)-2-甲基咪唑醋酸盐(DAIL-Ac)。并用核磁共振光谱(NMR)、傅里叶变换红外光谱(FTIR)、高分辨质谱(HRMS)等手段进行结构表征,表征测试结果表明所合成的两种离子液体结构正确,核磁图谱上几乎没有杂峰,推测其纯度达99%。用热重分析(TGA)考察其热稳定性,其中离子液体DAIL-Br具有较好的热稳定性,热分解温度为521.15 K。 2. 研究了双氨基功能化离子液体的水溶液体系对CO2吸收性能。研究结果表明,在303.15 K,100 kPa下,10%的DAIL-Br水溶液对CO2的饱和吸收量为1.05 mol CO2/mol IL。换算为质量吸收量,则为 18.5 wt %,这一结果高于目前文献报道的其他氨基功能化离子液体。 3. 在温度为353.15 K 和压力为0.2 kPa条件下,将吸收的CO2解吸出来。DAIL-Br吸收解吸循环4次后,吸收量基本保持不变,表明DAIL-Br具有良好的循环性能。 4. 以离子液体DAIL-Br为代表,根据FTIR和13C NMR等实验波谱分析结果提出了新型双氨基功能化离子液体对CO2的吸收机理,即2 mol -NH2与1 mol CO2反应发生化学反应,同时结合DFT量化计算进一步证明了提出的吸收机理的正确性。
Other AbstractCarbon dioxide is one of the main greenhouse gases,which is produced by the combustion of fossil fuel, such as coal, oil, and natural gas. The increasing of carbon dioxide leads to global warming and climate warming, brings serious damage to the ecological environment. This makes the capture and seperation of carbon dioxide becoming a new research hotspot. Ionic liquids have negligible vapor pressure, high thermal stability, which have the ability of the soluble or absorb carbon dioxide. Ionic liquids show a good prospect in the application of the absorbing of carbon dioxide, so the study of design and synthesis of new functionalized ionic liquids for CO2 capture is one of hot points on green chemistry and chemical engineering. The major work and innovative results for this dissertation are as follows. 1. Two novel dual amino-functionalized ionic liquids, 1,3-di (2′-aminoethylene)-2- methylimidazolium bromide (DAIL-Br) and 1,3-di (2′-aminoethylene)-2-methylimidazolium carbonate (DAIL-Ac) were designed and synthesized. Their structures were characterized by Nuclear Magnetic Resonance (NMR), Fourier Transform Infrared Spectroscopy (FTIR) and High Resolution Mass Spectrum (HRMS). The physic-chemical properties including thermal decomposition temperature, glass transition temperature and viscosity were determined. DAIL-Br has better thermal stability (its decomposition temperatures is 521.15 K). 2. CO2 absorption behaviors by aqueous solution of DAIL-Br at different temperatures and pressures were investigated in detail. The solubility of CO2 in aqueous solution of DAIL-Br (10%) at P0 = 100 kPa and temperature T = 303.15 K was 1.05 mol CO2/ mol IL. Calculated from the gravimetric aspect, the CO2 capture capacity of DAIL-Br is up to 18.5 wt %, which is obviously higher than previously reported task-specific ILs. 3. Ionic liquid cycle performances were also investigated. Upon heating the CO2 saturated solution of DAIL-Br at 353.15 K and 0.2 kPa, the captured CO2 could be released easily. The absorption capacities remain steady during four cycles of CO2 absorption and desorption. 4. The absorption mechanism was proposed though spectroscopic investigations (FTIR and NMR). What’s more, the mechanism involved was verified by density functional theory (DFT) calculations.
Document Type学位论文
Recommended Citation
GB/T 7714
张金芝. 新型双氨基功能离子液体的合成及碳捕集性能研究[D]. 中国科学院研究生院,2013.
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