化石燃料燃烧排放的CO₂被认为是导致全球变暖的主要原因，因此，减少CO₂排放对人类的持续发展至关重要。目前，醇胺吸收法是比较常用的CO₂吸收方法，但此方法存在易氧化降解、循环利用能耗高、对设备腐蚀性高等问题。季铵盐离子液体具有热稳定性高、蒸气压低、挥发性低、结构和性质可调变等特点，有望成为一种新型环保的CO₂吸收剂。

本文利用超声技术合成了6种季铵盐类离子液体，探讨了超声合成的最优工艺条件，通过测定和计算，分析了季铵盐类离子液体水溶液吸收CO₂的物性参数，研究了季铵盐类离子液体水溶液吸收CO₂的性能和机理。

主要工作如下：

(1) 季铵盐类离子液体的超声合成工艺条件探究

合成了6种季铵盐类离子液体N₂₂₂₄Mal、N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro和N₂₂₂₄Lys，探讨了超声强度、超声时间和搅拌速率对季铵盐离子液体产率的影响，发现超声法对提高离子液体产率和缩短合成时间效果明显，其中，对N₂₂₂₄Mal合成影响最显著。超声功率设定为400 W，经过超声时间1.0 h，N₂₂₂₄Mal的产率达到95.79%，能提高产率20.20%，缩短合成时间4.0 h。

(2) 季铵盐类离子液体的结构表征

通过红外光谱、核磁氢谱和核磁碳谱表征了6种季铵盐离子液体的结构，发现6种季铵盐离子液体的核磁共振图谱中H、C吸收峰的化学位移和数量与理论值相同，且6种季铵盐类离子液体的特征官能团的吸收峰均在红外光谱中对应出现，说明合成的6种季铵盐类离子液体与设计的结构相一致。

(3) 季铵盐类离子液体水溶液吸收CO₂的物性参数计算

在303-353 K范围，测定了6种离子液体的密度和粘度。发现随着温度升高，离子液体的密度和粘度都会减小。根据Glasser模型，计算了离子液体的标准熵和晶格能等物性参数。通过Eyring液体粘度理论，计算了离子液体的流动活化Gibbs自由能ΔG^*、流动活化焓ΔH^*和流动活化熵ΔS^*，发现焓效应决定其粘滞流动的阻力。此外，借助TG-DTG研究了离子液体的热稳定性，表明含氨基的离子液体N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro和N₂₂₂₄Lys，热稳定性较强。

通过“N₂O类比法”估算了CO₂在离子液体水溶液中的溶解度系数，发现随温度升高，CO₂的溶解度系数降低。计算了CO₂在离子液体水溶液中的扩散系数，顺序为：N₂₂₂₄Mal > N₂₂₂₄Lys > N₂₂₂₄Pro > N₂₂₂₄Sul > N₂₂₂₄Pyr > N₂₂₂₄Asp。

(4) 离子液体水溶液吸收CO₂的性能和机理研究

在303 K和浓度为0.5 mol L^-1的条件下，测定了离子液体水溶液对CO₂的吸收量，大小顺序为：N₂₂₂₄Lys > N₂₂₂₄Mal > N₂₂₂₄Pro > N₂₂₂₄Asp > N₂₂₂₄Pyr > N₂₂₂₄Sul，其中N₂₂₂₄Lys的吸收量最大为1.002 mol CO₂/mol IL。离子液体水溶液对CO₂的吸收量，随着温度和浓度升高而降低，随CO₂分压的升高而增加。6种离子液体水溶液经过5次吸收/解吸循环后，仍能保持初始吸收量的80%。

通过¹³C NMR谱图，发现N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro和N₂₂₂₄Lys的¹³C NMR谱图中均出现氨基甲酸酯特征峰，N₂₂₂₄Mal未出现。说明N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro和N₂₂₂₄Lys水溶液吸收CO₂为“zwitterion机理”，N₂₂₂₄Mal水溶液为物理吸收。此外，利用反应平衡热力学模型(RETM)，计算了离子液体水溶液吸收CO₂的热力学参数ΔH_sol和ΔS_sol。ΔH_sol都小于零，说明这5种离子液体水溶液吸收CO₂为放热过程。

CO₂ emissions from fossil fuel combustion are considered to be the main cause of global warming, therefore, reducing CO₂ emissions is essential of human sustainable development. Currently, alkanolamine absorption method is the more commonly used method for CO₂ absorption, but this method suffers from easy oxidative degradation, high energy consumption for recycling, and high corrosiveness to equipment. Quaternary ammonium-base ionic liquids have specific characteristics, for instance, high thermal stability, low vapor pressure, low volatility, as well as variable structure and properties, which are expected to be a new environmentally friendly CO₂ absorbent.

In this work, six quaternary ammonium -base ionic liquids were synthesized by ultrasound technology and the optimal process conditions for ultrasound synthesis were discussed. The physical parameters of CO₂ absorption into aqueous solutions of quaternary ammonium-base ionic liquids were analyzed by measurement and calculation. The performance and mechanism of CO₂ absorption into aqueous solutions of quaternary ammonium-base ionic liquids were investigated.

The main work is as follows:

(1) Exploration of ultrasonic synthesis process conditions for quaternary ammonium-base ionic liquids

Six quaternary ammonium based ionic liquids containing N₂₂₂₄Mal、N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro and N₂₂₂₄Lys were synthesized. The effects of ultrasonic intensity, ultrasonic time and stirring speed on the yield of ionic liquids were investigated. The ultrasonic method was found to be effective in improving the yield of ionic liquids and shortening the synthesis time, among which, the most significant effect was found on the synthesis of N₂₂₂₄Mal. When the ultrasonic power was set to 400 W, the yield of N₂₂₂₄Mal reached 95.79% after 1.0 h of ultrasonic time, which could increase the yield by 20.2% and reduce the synthesis time by 4 h.

(2) Structural characterization of quaternary ammonium-base ionic liquids

The structures of six quaternary ammonium base ionic liquids were characterized by ¹H NMR, ¹³C NMR, and FTIR. It was found that the chemical shifts and numbers of H and C absorption peaks in the NMR spectra of the six quaternary ammonium-base ionic liquids were all the same as the theoretical values. The absorption peaks of the characteristic functional groups of the six quaternary ammonium-base ionic liquids appeared in the infrared spectra correspondingly, which indicated that the six quaternary ammonium-base ionic liquids were consistent with the designed structures.

(3) Calculation of physical parameters for CO₂ absorption by quaternary ammonium-base ionic liquids aqueous solutions

The densities and viscosities of six ILs were measured in the temperature range of 303-353 K. It was found that the densities and viscosities of the ionic liquids decreased as the temperature increased. The physical parameters such as standard entropy and lattice energy of ionic liquids were calculated according to Glasser's model. The viscous fluid flow activation Gibbs free energy (ΔG*)，the viscous fluid flow activation enthalpy (ΔH*) and the viscous fluid flow activation entropy (ΔS*) of six ionic liquids were calculated by the Eyring liquid viscosity theory, which illustrated that the enthalpy effect determines their resistance to viscous flow. In addition, the thermal stabilities of ionic liquids were investigated by TG-DTG, which presented that the ionic liquids containing amino groups N₂₂₂₄Sul, N₂₂₂₄Pyr, N₂₂₂₄Asp, N₂₂₂₄Pro and N₂₂₂₄Lys had strong thermal stabilities.

The solubility coefficients of CO₂ into the ILs aqueous solutions were estimated by the "N₂O analogy method", and the CO₂ solubility coefficients were decreased with the increase of temperature. The diffusion coefficients of CO₂ into ILs aqueous solutions were calculated and the CO₂ diffusion coefficient order is: N₂₂₂₄Mal > N₂₂₂₄Lys > N₂₂₂₄Pro > N₂₂₂₄Sul > N₂₂₂₄Pyr > N₂₂₂₄Asp.

(4) Study on CO₂ absorption performance and mechanism by aqueous solutions of ILs

The CO₂ absorption capacities of ILs aqueous solutions were carried out at room temperature (303 K) and 0.5 mol L^-1, the CO₂ absorption showed the following order: N₂₂₂₄Lys > N₂₂₂₄Mal > N₂₂₂₄Pro > N₂₂₂₄Asp > N₂₂₂₄Pyr > N₂₂₂₄Sul, from which the maximum absorption of N₂₂₂₄Lys was 1.002 mol CO₂/mol IL. The CO₂ absorption of ILs aqueous solutions decreased with the increase of temperature and concentration, and promoted with the rise of CO₂ partial pressure. The ILs aqueous solutions were still maintain 80% of the initial absorption after 5 absorption/desorption cycles.

The characteristic peaks of carbamate appeared in the ¹³C NMR spectra of N₂₂₂₄Sul, N₂₂₂₄Pyr, N₂₂₂₄Asp, N₂₂₂₄Pro and N₂₂₂₄Lys, but no characteristic peak appeared in N₂₂₂₄Mal. The CO₂ absorption mechanism into N₂₂₂₄Sul, N₂₂₂₄Pyr, N₂₂₂₄Asp, N₂₂₂₄Pro and N₂₂₂₄Lys aqueous solutions followed the "zwitterion" absorption mechanism, while the N₂₂₂₄Mal aqueous solution was physical absorption. In addition, the thermodynamic parameters ΔH_sol and ΔS_sol of CO₂ absorption into ILs aqueous solutions were obtained by using the reaction equilibrium thermodynamic model (RETM) derivation. The ΔH_sol of N₂₂₂₄Sul、N₂₂₂₄Pyr、N₂₂₂₄Asp、N₂₂₂₄Pro and N₂₂₂₄Lys were less than zero, indicating that the CO₂ absorptions of these ILs aqueous solutions were exothermic processes. 

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