MEA/离子液体混合水溶液吸收CO_2的传质—反应机理
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摘要
温室气体引起的全球气候变暖已成为国际上关注的焦点。而C02作为最主要的温室气体,其控制与减排刻不容缓。一乙醇胺(MEA)化学吸收法是当今工业C02捕集应用最广泛吸收剂,具有吸收速率快、选择性良好等优势。论文研究的重点是基于传统MEA吸收法的基础上,通过离子液体的强化手段,提高混合体系的吸收容量,改善其抗氧化和再生能力,并降低再生能耗从而弥补传统MEA法的缺陷,使得强化后的吸收法更有利于工业应用与推广。论文选择MEA/离子液体混合水溶液吸收CO2的新体系,利用亲水性离子液体或实验室自行研发的高效功能性离子液体与MEA配比形成均一水溶液吸收C02,取得了以下的研究结果：
(1)对常规离子液体进行筛选后,发现MEA与1-丁基3-甲基-咪唑四氟硼酸钠([Bmim]BF4)这一混合体系具有良好的亲和性,具有较高的吸收负荷(0.447molCO2/mol absorbent)以及良好的抗氧化和再生能力；基于吸收-再生性能以及稳定性等评估考核,确定了MEA/[Bmim]BF4混合水溶液的最佳摩尔配比为7：3,并探讨了两组分在混合体系中的交互作用。
(2)结合有机胺“两性离子”反应机理以及混合溶液吸收特性考察结果,阐明了MEA/[Bmim]BF4混合水溶液体系吸收C02的机理,认为这一体系中仍然是MEA与C02的化学反应为主,并以[Bmim]BF4促进C02水解的反应为辅的耦合作用机制；建立了这一体系中C02的传质-反应动力学模型,确定了其吸收C02属拟一级快速反应；获得混合体系吸收C02过程的反应速率常数k2,mix为3487.6m3·kmol-1·s-1,离子液体促进CO2水解吸收的反应速率常数k2,IL为1936.7m3·kmol·s-1。
(3)由于常规离子液体对混合体系的吸收能力促进效果有限,因此合成了亲水性氨基酸功能性离子液体[C2OHmim][Gly]o这一功能性离子液体在室温下为固体,高温(80℃)下为液体；通过核磁共振分析,证实固体状态下的这一功能性离子液体无法直接与C02反应,溶解于有机溶剂也无法与C02反应,必须溶解于水中才能吸收CO2。相比于MEA以及MEA[Bmim]BF4混合水溶液,利用实验室合成的高效亲水功能性离子液体[C2OHmim][Gly]强化MEA吸收C02,在3%02浓度下还能保持较高的CO2吸收负荷(0.534molCO2mol absorbent),特别是在温度和氧气含量较高条件下,仍然具有较好的稳定性和抗氧化能力；同时也考察了MEA/[C2OHmim][Gly]混合溶液处理不同工艺工况条件烟气的吸收-再生特性。
(4)研究了MEA/[C2OHmim][Gly]混合水溶液吸收CO2的反应机理,发现MEA与[C2OHmim][Gly]这两种物质在水溶液中均遵循“两性离子”反应机理与C02进行反应,且随着混合体系中[C2OHmim][Gly]浓度的增加总反应速率常数增大；利用双膜理论建立了这一新体系的传质-反应动力学模型,获得了重要的动力学参数,MEA/[C2OHmim][Gly]混合体系吸收C02过程的总反应速率常数k2,mix为6506.4m3·kmol-1·s-1,[C2OHmim][Gly]吸收C02的反应速率常数k2.AAIL为8980.6m3·kmol-1·s-1.
本文也对比了MEA与这两类离子液体混合水溶液体系吸收C02的效果,证实利用亲水性离子液体以及功能性离子液体强化MEA的方法能有效保留MEA吸收C02反应速率快的特点,也能结合离子液体的稳定性增强体系的抗氧化能力,弥补MEA易降解、氧化的缺陷。其中[C2OHmim][Gly]功能性离子液对MEA法的强化效果更具优势。MEA/离子液体混合水溶液这一新C02捕集方法,将为目前亟待解决的C02控制与减排目标提供了新的思路,也为这一技术的进一步推广提供了基础数据与理论依据。
Monoethanolamine (MEA) is one of the most conventional absorbents for CO2capture from flue gas in the past few years and has still suffer several shortcomings. Herein, a mixed absorbent of MEA and ionic liquids was proposed to achieve CO2capture. The aim of the new system is to enhance the MEA process and obtain higher absorbtion capacity, antioxidant activity and regeneration efficiency. The hydrophilic ionic liquids used in this work were commercial-available or were synthesized in our laboratory. The main conclusions of this dissertation are:
(1) Screening from some conventional ionic liquids, it was found that the mixed solution of MEA and [Bmim]BF4have a highest absorption capacity compared with pure MEA aqueous. The optimum mole ratio of MEA to [Bmim]BF4was found to be7:3. The mixed absorbent owns higher stability and antioxidant activity compared with aqueous MEA solution in the present of8%O2. Additionally, the absorbent could be well recycled by thermal regeneration after multi-cycle experiments.
(2) Based on the zwitterions mechanism and the absorption results, the reaction mechanism of the CO2absorption into the mixed solution of MEA and [Bmim]BF4was clarified. The reaction between CO2and MEA was still the dominant reaction in the mixed absorbent solution. And,[Bmim]BF4has a positive effect on enhancing the hydration of CO2which could improve the whole absorption rate. The reaction rate constant k2k2,mix and k2,IL of the mixed solution of MEA/[Bmim]BF4were found to be3487.6m3·kmol·s-1and1936.7m3·kmol-1·s-1, respectively.
(3) A new hydrophilic amino acid ionic liquid ([C20Hmim][Gly]) that was functionalized based imidazolium ionic liquid with glycine anions and hydroxy group was designed for CO2absorption. Since [C20Hmim][Gly] is a solid at room temperature, chemical reaction between CO2and [C20Hmim][Gly] was occurring only in the presence of water. The absorption capacity of [C20Hmim][Gly] was0.575mol CO2/mol absorbent that was similar to the equimolar stoichiometry by the zwitterion mechanism. Furthermore,[C20Hmim][Gly] aqueous solution was mixed with MEA into aqucous solution for CO2capture, and the results showed a great intoxication ability and high regeneration efficiency compared with pure MEA solution, making the CO2capture by this mixture system more efficient and economic.
(4) The reaction mechanism of the CO2absorption into the mixed solution of MEA and [C2OHmim][Gly] was clarified. The mass transfer model of this system was established based on the membrane model and permeation model. Some important kinetic parameters such as the reaction rate constant and the enhancement factor were obtained. The reaction rate constant k2,mix and k2AAILs of the mixed solution of MEA/[C2OHmim][Gly] were found to be6506.4m3·kmol·s-1and8980.6m3·kmol·s-1, respectively.
The absorption and regeneration of the mixed solution of MEA/[Bmim]BF4and MEA/[C2OHmim][Gly] were contrast discussion. The results indicated that both the [Bmim]BF4and [C20Hmim][Gly] both could enhance the MEA process by great absorbtion capacity, good antioxidant activity and high regeneration efficiency. The results of this work will provide a new pathway for the CO2absorption and also will provide some theoretic data for the industrial application of this new technology.
(1)对常规离子液体进行筛选后,发现MEA与1-丁基3-甲基-咪唑四氟硼酸钠([Bmim]BF4)这一混合体系具有良好的亲和性,具有较高的吸收负荷(0.447molCO2/mol absorbent)以及良好的抗氧化和再生能力；基于吸收-再生性能以及稳定性等评估考核,确定了MEA/[Bmim]BF4混合水溶液的最佳摩尔配比为7：3,并探讨了两组分在混合体系中的交互作用。
(2)结合有机胺“两性离子”反应机理以及混合溶液吸收特性考察结果,阐明了MEA/[Bmim]BF4混合水溶液体系吸收C02的机理,认为这一体系中仍然是MEA与C02的化学反应为主,并以[Bmim]BF4促进C02水解的反应为辅的耦合作用机制；建立了这一体系中C02的传质-反应动力学模型,确定了其吸收C02属拟一级快速反应；获得混合体系吸收C02过程的反应速率常数k2,mix为3487.6m3·kmol-1·s-1,离子液体促进CO2水解吸收的反应速率常数k2,IL为1936.7m3·kmol·s-1。
(3)由于常规离子液体对混合体系的吸收能力促进效果有限,因此合成了亲水性氨基酸功能性离子液体[C2OHmim][Gly]o这一功能性离子液体在室温下为固体,高温(80℃)下为液体；通过核磁共振分析,证实固体状态下的这一功能性离子液体无法直接与C02反应,溶解于有机溶剂也无法与C02反应,必须溶解于水中才能吸收CO2。相比于MEA以及MEA[Bmim]BF4混合水溶液,利用实验室合成的高效亲水功能性离子液体[C2OHmim][Gly]强化MEA吸收C02,在3%02浓度下还能保持较高的CO2吸收负荷(0.534molCO2mol absorbent),特别是在温度和氧气含量较高条件下,仍然具有较好的稳定性和抗氧化能力；同时也考察了MEA/[C2OHmim][Gly]混合溶液处理不同工艺工况条件烟气的吸收-再生特性。
(4)研究了MEA/[C2OHmim][Gly]混合水溶液吸收CO2的反应机理,发现MEA与[C2OHmim][Gly]这两种物质在水溶液中均遵循“两性离子”反应机理与C02进行反应,且随着混合体系中[C2OHmim][Gly]浓度的增加总反应速率常数增大；利用双膜理论建立了这一新体系的传质-反应动力学模型,获得了重要的动力学参数,MEA/[C2OHmim][Gly]混合体系吸收C02过程的总反应速率常数k2,mix为6506.4m3·kmol-1·s-1,[C2OHmim][Gly]吸收C02的反应速率常数k2.AAIL为8980.6m3·kmol-1·s-1.
本文也对比了MEA与这两类离子液体混合水溶液体系吸收C02的效果,证实利用亲水性离子液体以及功能性离子液体强化MEA的方法能有效保留MEA吸收C02反应速率快的特点,也能结合离子液体的稳定性增强体系的抗氧化能力,弥补MEA易降解、氧化的缺陷。其中[C2OHmim][Gly]功能性离子液对MEA法的强化效果更具优势。MEA/离子液体混合水溶液这一新C02捕集方法,将为目前亟待解决的C02控制与减排目标提供了新的思路,也为这一技术的进一步推广提供了基础数据与理论依据。
Monoethanolamine (MEA) is one of the most conventional absorbents for CO2capture from flue gas in the past few years and has still suffer several shortcomings. Herein, a mixed absorbent of MEA and ionic liquids was proposed to achieve CO2capture. The aim of the new system is to enhance the MEA process and obtain higher absorbtion capacity, antioxidant activity and regeneration efficiency. The hydrophilic ionic liquids used in this work were commercial-available or were synthesized in our laboratory. The main conclusions of this dissertation are:
(1) Screening from some conventional ionic liquids, it was found that the mixed solution of MEA and [Bmim]BF4have a highest absorption capacity compared with pure MEA aqueous. The optimum mole ratio of MEA to [Bmim]BF4was found to be7:3. The mixed absorbent owns higher stability and antioxidant activity compared with aqueous MEA solution in the present of8%O2. Additionally, the absorbent could be well recycled by thermal regeneration after multi-cycle experiments.
(2) Based on the zwitterions mechanism and the absorption results, the reaction mechanism of the CO2absorption into the mixed solution of MEA and [Bmim]BF4was clarified. The reaction between CO2and MEA was still the dominant reaction in the mixed absorbent solution. And,[Bmim]BF4has a positive effect on enhancing the hydration of CO2which could improve the whole absorption rate. The reaction rate constant k2k2,mix and k2,IL of the mixed solution of MEA/[Bmim]BF4were found to be3487.6m3·kmol·s-1and1936.7m3·kmol-1·s-1, respectively.
(3) A new hydrophilic amino acid ionic liquid ([C20Hmim][Gly]) that was functionalized based imidazolium ionic liquid with glycine anions and hydroxy group was designed for CO2absorption. Since [C20Hmim][Gly] is a solid at room temperature, chemical reaction between CO2and [C20Hmim][Gly] was occurring only in the presence of water. The absorption capacity of [C20Hmim][Gly] was0.575mol CO2/mol absorbent that was similar to the equimolar stoichiometry by the zwitterion mechanism. Furthermore,[C20Hmim][Gly] aqueous solution was mixed with MEA into aqucous solution for CO2capture, and the results showed a great intoxication ability and high regeneration efficiency compared with pure MEA solution, making the CO2capture by this mixture system more efficient and economic.
(4) The reaction mechanism of the CO2absorption into the mixed solution of MEA and [C2OHmim][Gly] was clarified. The mass transfer model of this system was established based on the membrane model and permeation model. Some important kinetic parameters such as the reaction rate constant and the enhancement factor were obtained. The reaction rate constant k2,mix and k2AAILs of the mixed solution of MEA/[C2OHmim][Gly] were found to be6506.4m3·kmol·s-1and8980.6m3·kmol·s-1, respectively.
The absorption and regeneration of the mixed solution of MEA/[Bmim]BF4and MEA/[C2OHmim][Gly] were contrast discussion. The results indicated that both the [Bmim]BF4and [C20Hmim][Gly] both could enhance the MEA process by great absorbtion capacity, good antioxidant activity and high regeneration efficiency. The results of this work will provide a new pathway for the CO2absorption and also will provide some theoretic data for the industrial application of this new technology.
引文
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