醇胺法CO2吸收剂新型降解抑制剂及动力学研究
文献类型：学位论文
| 作者 | 赵志军 |
| 学位类别 | 博士 |
| 答辩日期 | 2014-04 |
| 授予单位 | 中国科学院研究生院 |
| 导师 | 张香平 |
| 关键词 | 降解 CO2吸收 抑制剂 离子液体 乙醇胺 动力学 |
| 其他题名 | Study of novel degradation inhibitors and its kinetics for CO2 capture with monoethanolamine absorbent |
| 学位专业 | 化学工艺 |
| 中文摘要 | 目前最具工业应用潜力的烟气CO2捕集方法是一乙醇胺(MEA)吸收法，其具有操作简单、技术成熟和吸收速度快等优点，缺点是再生能耗高以及吸收剂容易降解等。据统计因降解损失的费用占到了操作成本的10%左右，针对这些问题，本论文开展了新型有机胺降解抑制剂的研究，具体成果如下： （1） 设计、制作、建立了降解抑制实验评价装置，其特点是能够进行封闭连续 实验，可避免MEA溶液在实验条件(MEA溶液浓度为3.3～7.5mol/L，纯氧，温度范围40～120°C，操作压力范围为250～1000kPa，加入抑制剂浓度为0.05mol/L)随气泡夹带流失造成的误差。 （2） 考察了系列无机抑制剂如亚硫酸钠、酒石酸钾钠和系列有机抑制剂，比 如2-硫苏糖醇、苏糖醇、EDTA等的抑制降解效果。通过实验筛选出了抑制性能最好的是酒石酸钾钠。对酒石酸钾钠进行了系统研究，考察了温度、氧气分压、酒石酸钾钠浓度对MEA降解性能的影响，得到了在加入酒石酸钾钠后MEA溶液的降解动力学模型。结果表明温度是影响降解的主要因素，氧气分压对抑制性能的影响较小。其它实验条件相同时，温度越高，酒石酸钾钠浓度越高，抑制MEA降解的性能越明显。 （3） 设计、合成和表征了两种阴阳离子均具有抑制作用的离子液体型抑制剂 MTA和HTA，在同样的实验条件下比较了其与其它典型抑制剂的效果。实验结果表明，加入抑制剂后，MEA的降解速度减慢。随着温度或压力升高，降解速度加快，其中温度对降解速度的影响更明显。所考察的系列抑制剂在无负载CO2时的抑制顺序是：MTA > 酒石酸钾钠 ＞ HTA ＞ 亚硫酸钠。 （4） 对筛选出来的MTA进行了系统研究，在MEA浓度范围3.3～5.0 kmol/m3, P(O2)范围150～350 kPa，反应温度为55～120 °C，MTA加入量为0～0.1mol/L，Fe2+浓度范围0.2～1.0 mM，CO2负载量为0.2～0.4 mol/mol?MEA，反应时间为75 h的实验条件下进行了七因素三水平的正交试验。获得了加入离子液体抑制剂MTA后MEA溶液降解的动力学模型。 （5） 离子液体进入大规模应用，其自身的降解性能是关键因素之一，本文采用 所建立的实验装置和方初步研究了pH值对离子液体[Bmim][Cl]降解性能的影响及降解机理。 |
| 英文摘要 | The most effective and widely used techniques to capture CO2 from low-pressure flue gas are chemical adsorption using alkanolamines solutions. The most widely used alkanolamines solutions is monoethanolamine (MEA) because it is very reactive and thus is able to treat a high volume of acid gas removal at a fast rate. However, it also suffers disadvantages like a high requirement for CO2 regeneration, low CO2 loading capacity and solvent degradation. The solvent degradation is estimated to be around 10% of the total cost of CO2 capture (Rao and Rubin 2002). Therefore, developing new degradation inhibitors with high efficiency is urgently needed. The major work and innovative results for this dissertation are summarized as follows. (1) The continuous apparatus was made firstly which could avoid the error caused by MEA volatilization. Then the degradation experiment were conducted in a sealed reactor with 100% O2 using aqueous (MEA) concentration from 3.3 to 7.5 mol/L in the absence of CO2, the concentration of the inhibitor is 0.05 mol/L. The temperature varies from 40 to 120 °C and the O2 pressure from 250 to 1000 kPa. (2) The Several inorganic inhibitors, i. e., sodium sulfite (Na2SO3), potassium sodium tartrate tetrahydrate (KNaC4H4O6) and organic inhibitors like dithiothreitol (C4H10O2S2), meso-erythritol (C4H10O4), and ethylenediaminetetraacetic acid (EDTA) are investigated too. The result showed the most effective inhibitors is KNaC4H4O6. Then the degradation kinetics of MEA solution with KNaC4H4O6 inhibitor was studied systematically under conditions such as degradation temperature, the O2 pressure and the concentrations of KNaC4H4O6. The experimental results showed that the influence of the O2 pressure is smaller than the temperature. Under the same experimental conditions, the higher the temperature is the more the degradation is while the high the concentration of KNaC4H4O6 the less the degradation is. (3) Two novel ionic liquid (IL) degradation inhibitors, Monoethanolamine tartrate (MTA) and mercapto-ethylamine tartrate (HTA) were designed, synthesized and characterized. Under the same experimental condition, their inhibition ability were compared with other typical inhibitors. The results suggested that the increases of temperature or pressure lead to an increase of the MEA degradation rate, but the influence of the pressure is smaller than the temperature. Among all the inhibitors, the most effective inhibitor is MTA. The results indicated that the inhibity extent is in the order: MTA > KNaC4H4O6 > HTA > Na2SO3. (4) The degradation orthogonal experiment of MEA solution with MTA was studied under condition typical of the CO2 absorption process considering key factors, such as aqueous (MEA) concentration from 3.3 to 7.5 mol/L, the O2 pressure from 150 to 300 kPa, the temperature varies from 55 to 120 °C, the MTA concentration from 0.025 to 1.0 mol/L, the Fe2+ concentration from 0.2-1.0 mM, and the CO2 loading from 0.2-0.4 mol/mol?amine. The degradation kinetic model of MEA solution which firstly introduces the influences of the components of MTA and Fe2+ was proposed by fitting the experimental data. (5) The ionic liquid has potential use in large-scale application in which its degradaton ablity is one key fator involved. And then the degradaiton mechanisum of ionic liquid [Bmim][Cl] and the effect of pH value on degradation was studied with our experiment aparratus and methods in this study. |
| 语种 | 中文 |
| 公开日期 | 2015-07-08 |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/15528]  |
| 专题 | 过程工程研究所_研究所（批量导入） |
| 推荐引用方式 GB/T 7714 | 赵志军. 醇胺法CO2吸收剂新型降解抑制剂及动力学研究[D]. 中国科学院研究生院. 2014. |
入库方式： OAI收割
来源：过程工程研究所
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