基于胺基咪唑功能离子液体吸收分离CO_2性能的研究
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摘要
燃煤过程中以CO_2为主的温室气体的排放，引起全球变暖的现实正不断地向全世界敲响警钟。胺基咪唑功能离子液体在吸收分离CO_2方面具有高效、经济、环保等方面的优势，是一种极具竞争潜力的CO_2分离固定技术。然而，胺基咪唑功能型离子液体固有的高粘度特性极大地影响了其吸收分离CO_2的性能，从而阻碍了该项技术的大规模应用。因此，研究探索一种能够有效改善胺基咪唑功能型离子液体吸收分离CO_2性能的方法，对于该项技术在燃煤CO_2减排领域的应用具有十分重要的理论和应用价值。
本文选择了具有相对较低粘度和较高CO_2吸收性能的1-(1-胺乙基)-3-甲基咪唑氟硼酸盐([NH_2e-mim][BF_4])为研究对象，重点对其合成制备方法、改善[NH_2e-mim][BF_4]在CO_2吸收分离过程中的传质性能、吸收剂物化性质的估算及其与CO_2吸收性能之间的关联预测等进行了系统研究，主要内容包括：
运用“两步合成法”成功合成了[NH_2e-mim][BF_4]，并系统全面地研究了反应温度、反应时间、溶剂种类、提纯条件、不同阴离子置换剂等对胺基咪唑功能离子液体的合成产率、产物纯度和合成成本的影响，得到了合成制备[NH2-emim][BF_4]的两步反应的最佳工艺条件和原料选取的原则。
采用功能型离子液体与醇胺混合以及与常规离子液体混合的方法，对改善胺基咪唑功能离子液体[NH_2e-mim][BF_4]在CO_2中的吸收分离性能进行了有益的尝试，通过实验得到了基于较优CO_2吸收和解析性能的混合物配比、吸收和解析工艺条件及多次吸收-解析循环中混合物的物化性能变化。研究结果表明，[NH_2e-mim][BF_4]在与醇胺和常规离子液体混合后均极大地降低了其粘度，有效地改善了其CO_2的吸收分离性能，[NH_2e-mim][BF_4]与常规离子液体的混合较其与醇胺的混合在吸收分离CO_2的性能的改善上更具优势。
借助已有的物化性质估算方法对基于[NH_2e-mim][BF_4]的两种混合体系的物化性质进行了估算，并研究分析了其与吸收分离CO_2性能之间的关系。研究显示，运用所估算的物化性质参数能为混合体系吸收分离CO_2的性能差异提供微观解释，同时也可以较好地预测分析温度、物质的组成等对两类混合体系吸收分离CO_2的性能的影响。
Global warming is caused by greenhouse gas emission, particularly by a large amountof CO_2released into the atmosphere from coal combustion, and this issue continues toreceive worldwide attention. Amino imidazole functional ionic liquids has high efficiency,economy, environmentally friendly and other advantages in the absorption separation ofCO_2, is a highly competitive potential CO_2emission reduction technology. However, highviscosity characteristics of amino imidazole functional ionic liquids hindered the masstransfer of CO_2absorption, greatly influenced the absorption performance, and limited thelarge-scale application of the technology. So, it is very important and necessary to explorean effective way on improving CO_2absorption and separation performance of aminoimidazole functional ionic liquids, which has important theoretical and application value forthe application in the field of CO_2emission reduction in flue gas.
1-(1-aminoethyl)-3-methyl imidazole tetrafluoroborate ([NH_2e-mim][BF_4]) waschoosen which had lower viscosity and higher CO_2absorption performance as therepresentative of amino imidazole functional ionic liquids in this paper. Methods ofsynthesis and possible ways on improving the gas-to-liquid mass transfer between CO_2with[NH_2e-mim][BF_4] were studied. Then the absorbent physicochemical properties wereestimated, and the relationship with CO_2absorption performance were discussed. The maincontents were as follows:
[NH_2e-mim][BF_4] was synthesized successfully by "two step synthesis" method. Andthe effect of reaction temperature，reaction time，solvent type，purification conditions anddifferent anion exchange agents on the yield、the purity and the economy were discussedsystematically and comprehensively. The optimum process conditions of two step reactionsand the principle of material selection were obtained.
An useful attempt were be carried out to improve CO_2absorption and separationperformance of [NH_2e-mim][BF_4] by mixing with alcohol amine and conventional ionicliquid. Suitable ratio and optimal conditions of CO_2absorption and regeneration, and thechanges of physical and chemical properties of mixtures after multiple absorption- desorption were obtained by experiment. The results showed that the viscosity of two kindof mixtures were reduced dramatically, and the CO_2absorption and separation performancewere improved effectively comparing with [NH_2e-mim][BF_4]. It had more advantage that[NH_2e-mim][BF_4] blended with conventional ionic liquids than mixed with alcohol aminefor achieving better CO_2absorption and separation performance.
Physical and chemical properties of two kinds of hybrid system based on[NH_2e-mim][BF_4] were estimated using existing methods, and the relationship betweenphysicochemical properties and CO_2absorption and separation performance were discussed.Studies have shown that the use of the estimated parameters of the physical and chemicalproperties can provide a microscopic explanation on the CO_2absorption and desorptionperformance difference for the mixed systems. At the same time, it also can be used topredict the effects of temperature and material composition of two kind of hybrid system onCO_2absorption and separation performance.
本文选择了具有相对较低粘度和较高CO_2吸收性能的1-(1-胺乙基)-3-甲基咪唑氟硼酸盐([NH_2e-mim][BF_4])为研究对象，重点对其合成制备方法、改善[NH_2e-mim][BF_4]在CO_2吸收分离过程中的传质性能、吸收剂物化性质的估算及其与CO_2吸收性能之间的关联预测等进行了系统研究，主要内容包括：
运用“两步合成法”成功合成了[NH_2e-mim][BF_4]，并系统全面地研究了反应温度、反应时间、溶剂种类、提纯条件、不同阴离子置换剂等对胺基咪唑功能离子液体的合成产率、产物纯度和合成成本的影响，得到了合成制备[NH2-emim][BF_4]的两步反应的最佳工艺条件和原料选取的原则。
采用功能型离子液体与醇胺混合以及与常规离子液体混合的方法，对改善胺基咪唑功能离子液体[NH_2e-mim][BF_4]在CO_2中的吸收分离性能进行了有益的尝试，通过实验得到了基于较优CO_2吸收和解析性能的混合物配比、吸收和解析工艺条件及多次吸收-解析循环中混合物的物化性能变化。研究结果表明，[NH_2e-mim][BF_4]在与醇胺和常规离子液体混合后均极大地降低了其粘度，有效地改善了其CO_2的吸收分离性能，[NH_2e-mim][BF_4]与常规离子液体的混合较其与醇胺的混合在吸收分离CO_2的性能的改善上更具优势。
借助已有的物化性质估算方法对基于[NH_2e-mim][BF_4]的两种混合体系的物化性质进行了估算，并研究分析了其与吸收分离CO_2性能之间的关系。研究显示，运用所估算的物化性质参数能为混合体系吸收分离CO_2的性能差异提供微观解释，同时也可以较好地预测分析温度、物质的组成等对两类混合体系吸收分离CO_2的性能的影响。
Global warming is caused by greenhouse gas emission, particularly by a large amountof CO_2released into the atmosphere from coal combustion, and this issue continues toreceive worldwide attention. Amino imidazole functional ionic liquids has high efficiency,economy, environmentally friendly and other advantages in the absorption separation ofCO_2, is a highly competitive potential CO_2emission reduction technology. However, highviscosity characteristics of amino imidazole functional ionic liquids hindered the masstransfer of CO_2absorption, greatly influenced the absorption performance, and limited thelarge-scale application of the technology. So, it is very important and necessary to explorean effective way on improving CO_2absorption and separation performance of aminoimidazole functional ionic liquids, which has important theoretical and application value forthe application in the field of CO_2emission reduction in flue gas.
1-(1-aminoethyl)-3-methyl imidazole tetrafluoroborate ([NH_2e-mim][BF_4]) waschoosen which had lower viscosity and higher CO_2absorption performance as therepresentative of amino imidazole functional ionic liquids in this paper. Methods ofsynthesis and possible ways on improving the gas-to-liquid mass transfer between CO_2with[NH_2e-mim][BF_4] were studied. Then the absorbent physicochemical properties wereestimated, and the relationship with CO_2absorption performance were discussed. The maincontents were as follows:
[NH_2e-mim][BF_4] was synthesized successfully by "two step synthesis" method. Andthe effect of reaction temperature，reaction time，solvent type，purification conditions anddifferent anion exchange agents on the yield、the purity and the economy were discussedsystematically and comprehensively. The optimum process conditions of two step reactionsand the principle of material selection were obtained.
An useful attempt were be carried out to improve CO_2absorption and separationperformance of [NH_2e-mim][BF_4] by mixing with alcohol amine and conventional ionicliquid. Suitable ratio and optimal conditions of CO_2absorption and regeneration, and thechanges of physical and chemical properties of mixtures after multiple absorption- desorption were obtained by experiment. The results showed that the viscosity of two kindof mixtures were reduced dramatically, and the CO_2absorption and separation performancewere improved effectively comparing with [NH_2e-mim][BF_4]. It had more advantage that[NH_2e-mim][BF_4] blended with conventional ionic liquids than mixed with alcohol aminefor achieving better CO_2absorption and separation performance.
Physical and chemical properties of two kinds of hybrid system based on[NH_2e-mim][BF_4] were estimated using existing methods, and the relationship betweenphysicochemical properties and CO_2absorption and separation performance were discussed.Studies have shown that the use of the estimated parameters of the physical and chemicalproperties can provide a microscopic explanation on the CO_2absorption and desorptionperformance difference for the mixed systems. At the same time, it also can be used topredict the effects of temperature and material composition of two kind of hybrid system onCO_2absorption and separation performance.
引文
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