醇胺溶液富集CO_2的研究
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摘要
二氧化碳(CO_2)排放问题所引起的温室效应是目前亟待解决的课题。以矿物燃料为主的火电厂是CO_2的一个集中排放源,排放出的CO_2量超过排放总量的30%,若能对其烟道气中CO_2进行回收利用,则是一项既有良好社会效益又有经济效益的工作。采用醇胺溶液回收中低浓度CO_2是一种传统的方法,也是最为经济的方法。本论文以制定更有效的吸收剂配方为目标进行了初步工作,为更深入开展这方面的研究建立了合理的实验方法,同时积累了必要的、有参考价值的实验数据。
     本文对AEE、AMP单组分溶液吸收CO_2的吸收情况进行了考察;研究了CO_2浓度与单组分溶液pH的对应关系,探讨了通过pH值法测定溶液中CO_2浓度的可行性。实验结果表明:AEE作为一种新型CO_2吸收剂,具有吸收速率快、吸收量大以及对温度变化不敏感等优点,具有很高的研究价值;醇胺溶液中CO_2浓度在一定范围内,溶液pH值的变化与CO_2浓度的变化成线性对应关系,可用方程pH=-IX+J来表示。
     对总胺浓度为40%(质量百分比)的AEE+MDEA和AEE+AMP溶液吸收CO_2的吸收效果进行了考察,测定了溶液吸收CO_2的吸收速率与吸收时间和吸收量的变化关系。总结认为两种体系的吸收液均表现出良好的吸收性能,适合工业应用,并分别考察了不同温度下吸收速率的变化。
     探讨了AEE与MDEA混合溶液在吸收过程中的交互作用。结果表明:在MDEA溶液中加入一定量的AEE,可以有效地提高体系吸收CO_2的性能,在摩尔吸收比低于0.5时,溶液中AEE摩尔浓度每增加10%,E相应增加约20%,AEE+MDEA体系溶液在一定的摩尔吸收比的条件下存在交互作用,且交互系数随体系的摩尔吸收比的增加而降低。
     在磁力搅拌恒温加热的再生装置中,对醇胺溶液吸收CO_2富液再生性能进行考察。结果表面:饱和的吸收液可以通过加热的方法进行再生,再生后的溶液可以继续吸收CO_2,其中20%AEE+20%MDEA体系溶液经过四次吸收与解吸以后的解吸率可以达到99%。
Greenhouse effect induced by the emissions of carbon dioxide(CO_2)has been the most serious issue to be solved recently.Fossil fuel-based thermal power plant is a concentrated source of CO_2 emissions,and it contains more than 30 percent of the total amount of CO_2 emissions.If the CO_2 containing fuel gas can be recovered,it would be beneficial both socially and economically.Using alcohol amine solution to absorption CO_2 is a traditional and the most economical method.This article conducted preliminary experiments in order to develop more effective absorbents and accumulate necessary and valuable experimental data.
     The single component solution of AEE(or AMP)for CO_2 absorption was investigated, and then the relationship between CO_2 concentration and the pH of solution was also studied, finally,the possibility of measuring CO_2 concentration by the method of pH was discussed. Experimental results showed that AEE as a new type of CO_2 absorbers was worth to be studied.It had advantages of fast absorption rate、high absorption capacity and insensitiveness to temperature changes.When the CO_2 concentration within a limitted range in the alcohol amine solution,the pH value of the solution changed linearly with the CO_2 concentration change,which can be expressed by the equation of pH=-IX+J.
     Absorption rates of gaseous CO_2 with absorption time and absorption capacity were measured in a 40%(wt)alcohol amine concentration aqueous of AEE and MDEA or AEE and AMP.And the absorption rates of the solutions at different temperatures were measured. It was found that both of the two systems showed good absorption properties,they are suitable for industrial applications.
     The interaction between AEE and MDEA mixed solution in the absorption process.The results show that addition of AEE could effectively improve the CO_2 absorption performance of the MDEA solution.When the tool absorption rate less than 0.5,the factor of E increased by about 20%with the increment of AEE content by 10%.There will be interactions in one certain mol absorptance rate of the AEE+MDEA system,and the interaction coefficient decrease with the mol absorptance rate increase.
     In order to improve the efficiency of the CO_2 cycling process and to reduce the regeneration energy consumption,it is necessary to investigate the regeneration behavior of the saturated alcohol amine solution.Results showed that saturated solution can be renewed through the method of being heating,the renewed solution could reabsorb CO_2.The 20%AEE+20%MDEA system's desorption rate reached 99%after four absorptions and desorptions cycles.
引文
[1]董尧清,郭一君.二氧化碳排放与中国发动机工业的任务.现代车用动力,2008,2(1):6-10.
    [2]马骏.膜接触器分离混合气中二氧化碳的研究:(硕士学位论文).南京:南京理工大学,2004.
    [3]文继英,李青霞.全球变暖问题浅探.科协论坛,2007,4(2):355-356.
    [4]Donald J.Wuebbles,Atul K.Jain.Concerns about climate change and the role of fossil fuel use.Fuel Process Technol,2001,71(1-3):99-119.
    [5]马一太,魏东,吕灿仁.温室气体减排与CO_2资源化宏观研究与探讨.大连理工大学学报,2001,11(41):9-14.
    [6]陈长虹,鲍仙华.全球能源消费与CO_2排放量.上海环境科学,1999,18(2):62-64.
    [7]IPCC.Climate Change 2000.Cambridge:Cambridge University Press 2000.
    [8]高峰,孙成权,曲建升.全球气候变化研究的新认识-IPCC第三次气候评价报告第一工作组报告概要.地球科学进展,2001,16(3):442-445.
    [9]高峰,孙成权,曲建升.气候变化对自然和人类社会系统的影响-IPCC第三次气候变化评价报告:第二工作组报告概要.地球科学展,2001,16(4):590-592.
    [10]高峰,孙成权,曲建升.气候变化减缓的战略措施-IPCC第三次气候变化评价报告:第三工作组报告概要.地球科学进展,2002,17(1):132-134.
    [11]董尧清,郭一君.二氧化碳排放与中国发动机工业的任务.现代车用动力,2008,129(1):6-10.
    [12]中华人民共和国国家统计局.中国统计年年鉴-2003.北京:中国统计出版社,2003.
    [13]吴克明,黄松荣,Concha F.温室气体CO_2的分离回收及其资源化.武汉科技大学学报(自然科学版),2001,24(4):365-369.
    [14]C.Mustacchi,P.Armenante,V.Cena.Carbon Dioxide Removal from Power Plans Exhaust.Environment International,1979,2(4-6):453-456.
    [15]D.S.Arnold,D.A.Barren,R.H.Isom.CO_2 can be Produced form Flue Gas of Conventional,Fossil-Fuel-Fired Power Plants.Environmental Progress,1994,139(3):214-219.
    [16]Tomio Mimura,Hidenobu Simayoshi,Taiichiro Suda et al.Development of Energy Saving Technology for Fuel Gas Carbon Dioxide Recovery in Power Plant by Chemical Absorption Methods and Steam System.Energy Convers.Mgmt,1997,38(1):57-62.
    [17]夏明珠,严莲荷,雷武等.二氧化碳的分离回收技术与综合利用.现代化工,1999,19(5):46-48.
    [18]Colin L Leci.Development Requirements for Absorption Processes for Effective CO_2Capture from Power Plants.Energ Convers.Mgmt,1997,38(1):45-50.
    [19]A.Chakma,A.K.Mehrotra,B.Nielsen.Comparison of Chemical Solvents for Mitigating CO_2Emissions from Coal-fired Power Plants.Heat Recovery System & CHP,1995,15(2):231-240.
    [20]张美华.二氧化碳生产及应用.西安:西北大学出版社,1988.
    [21]李天成.二氧化碳处理技术现状及其发展趋势.化学工与工程,2002,19(2):17-20.
    [22]黄建彬.工业气体手册.北京:化学工业出版社,2001.
    [23]李基涛,张伟德,区泽棠.掺入CO催化活化CO_2加氢合成甲醇的研究.环境污染与防治,1998,20(5):15-18.
    [24]闫志勇,张虹.CO_2排放导致的地球温升问题及基本技术对策.环境科学进展.1999,7(6):175-181.
    [25]二氧化碳的资源与利用.化工开发与设计,2000(3):31-38.
    [26]李天成.二氧化碳处理技术现状及其发展趋势.化学工业与工程,2002,19(2):17-20.
    [27]李成文.注二氧化碳提高原油采收率.国外油田工程,1994,10(6):1-3.
    [28]王德权,张铭.从油田自备热电厂回收CO_2以提高原油采收率及改善生态环境.国外油田工程,1999,15(7):8-9.
    [29]钟战铁.混合胺溶液吸收CO_2气体的初步研究:(硕士论文).杭州:浙江大学,2002.
    [30]叶愈权,陈全福.二氧化碳分离技术.上海:上海交通大学出版社,1990.
    [31]王松汉.石油化工设计手册,第3卷化工单元过程.北京:化学工业出版社,2001.
    [32]P.H.M.Feron,A.E.Jansen.The Production of Carbon Dioxide from Flue Gas by Membrane Gas Absorption.Energy convers.Mgmt.1997,38(1):93-98.
    [33]张阿玲,方栋主.温室气体CO_2的控制和回收利用.中国环境科学出版社,北京:1996.
    [34]任建新.膜分离技术及其应用.北京:化学工业出版社.2003:4-5
    [35]郑领英,王学松.膜技术.北京:化学工业出版社.2000:6
    [36]黄肖容,隋贤栋,张学斌.用梯度硅藻土膜分离CO_2/N_2混合气.天然气化工.2002,27(1):9-13.
    [37]秦向东,温铁军,金美芳.脱除与浓缩二氧化碳的膜分离技术.膜科学与技术.1998,18(6):7-13
    [38]甄寒菲,王志,李保安等.用于分离CO_2的高分子膜.高分子材料科学与工程.1999,15(6):29-31
    [39]VOROBER A V,KHIM T O.Recent advance in CO_2 separation.Technol.1985,19(4):544.
    [40]甄寒菲,王志,李保安等.用于分离CO_2的高分子膜.高分子材料科学与工程,1999,15(6):29-31.
    [41]张学模,储政,古俊智.脱CO_2技术进展及评价.化学工业与工程技术,2001,22(2):14-23.
    [42]Astarita G,Savage D W,Bisio A.Gas Treating with Chemical Solvents.New York:John Wiley & Sons,1983.
    [43]Rinker E.B.,Ashour S.S.,Sandall O.C.Absorption of Carbon Dioxide into Aqueous Blends of Diethanolamine and Methyldiethanolamine.Ind.Eng.Chem.Res.2000,39(11),4346-4356.
    [44]陈甘棠.化学反应工程.北京:化学工业出版社,1995:170-181.
    [45]马友光,宋宝东.界面性质对气液传质的影响.化学工程,1997,(4):6-2.
    [46]Haruo Hikita,Satoru Asai,Yoshio Katsu,et al.Absorption of carbon dioxide into aqueous monoethanolamine solutions.Chem.Eng.Sci.,1979,25(5):793-800.
    [47]八田四郎次.吸收发展史.化学工学,1963,271(11):843-846.
    [48]只木祯力,前猫四郎.对湿壁塔内液膜内的研究.化学工学,1963,27(2):66-73.
    [49]寺本正奖.NaSO_3水溶液对SO_3和CO_2的同时吸收.化学工学,1978,42(6):312-316.
    [50]E.Sada,H.Kumazawa,M.A.Butt.Solubility and diffusivity of gases in aqueous solutions of amines.J.Chem.Eng.1978,23(2):161-163.
    [51]董吉川.醇胺吸收二氧化碳的研究(硕士论文).哈尔滨:哈尔滨工程大学,2000.
    [52]天津大学物理化学教研室主编.物理化学.高等教育出版社,1996:170-182.
    [53]C.A卡捷也夫.动力学在金属学中的应用(王仁智译).国防工业出版社,1959:7-81.
    [54]庞贻慧.物理化学.人民卫生出版社,1990:135-434.
    [55]Adamsan A.W.表面的物理化学(顾惕人译).北京:科学出版社,1984:245-247.
    [56]陈甘棠.化学反应工程.化学工业出版社,1995:170-181.
    [57]马友光,白鹏,余国琼.气液传质理论研究进展.化学工程,1996(6):7-10.
    [58]Michael Caplow.Kinetics of carbamate formation and breakdown.J.Am.Chem.Soc.1968,90(24):6795-6803.
    [59]P.V.Danckwerts.The reactions of CO_2 with ethanolamines.Chem.Eng.Sci.1979,34(4):443-446.
    [60]G.F.Versteeg,W.P.M.van Swaaij.On the kinetics between CO_2 an alkanolamines both in aqueous and non-aqueous solutions-Ⅰ.Primary and Secondary amines.Chem.Eng.Sci.,1988,43,(3):573-585.
    [61]Erik Jorgensen,Carl Faurhold.Reactions between Carbon Dioxide and Amine Alcohols.Acta Chem.Scand.1954,8(7):1141-1144.
    [62]G.F.Versteeg,W.P.M.van Swaaij.On the kinetics between CO_2 an alkanolamines both in aqueous and non-aqueous solutions-Ⅱ.Tertiary amines.Chem.Eng.Sci.1988,43(3):587-591.
    [63]Terrence L.Donaldson,Yen N.Nguyen.Carbon dioxide reaction and transport in aqueous amine membranes,Ind.Eng.Chem.Fundam.1980,19(3):260-266.
    [64]Jong Sup Lee,Sung Chan Nam,Jae Ek Son,et al.Solubility of CO_2 in Aqueous MethyldiethanolamineSolutions,J.Chem.Eng.Data,1997,42(6):1161-1164.
    [65]刘华兵,徐国文,张成芳等.活化MDEA水溶液中二氧化碳溶解度,华东理工大学学报,1999,25(3):242-246.
    [66]Hani A.Al-Ghawas,Daniel P.Hagewiesche,Gabriel Ruiz-Ibanez,et al.Physicochemical Properties Important for Carbon Dioxide Absorption in Aqueous Methyldiethanolamine.J.Chem.Eng.Data.1989,34(4):385-391.
    [67]Rowley R.L.,Adams M.E.,Marshall T,L.,et al.Measurement of Diffusion Coefficients Important in Modeling the Absorption rate of Carbon Dioxide into Aqueous N-Methyldiethanolamine.J.Chem.Eng.Data.1997,42(2):310-317.
    [68]H.Bosch,G.F.Versteeg,W.P.M.Van Swaaij.Gas-Liquid mass transfer with parallel reversible reactions-Ⅰ Absorption of CO_2 into solutions of sterically hindered amines.Chem.Eng.Sci.1989,44(11):2723-2734.
    [69]David A.Glasscock,Gary T.Rochelle,Numerical Simulation of Theories for Cas Absorption with Chemical Reaction,AlChe.J.,1989,35(8):273-278.
    [70]S.S.Laddha,J.M.Diaz,P.V.Danckwerts.The N_2O analogy:the solubilities of CO_2 and N_2O in aqueous solutions of organic compounds.Chem.Engng.Sci.,1981,36(1):228-229.
    [71]Eizo Sada,Hidehiro Kumazawa,M.A.Butt.Solubility and diffusivity of gases in aqueous solutions of amines.J.Chem.Eng.Data.1978,23(2):161-163.
    [72]Fang-Yuan Jou,A.E.Mather,F.D.Otto.The solubility of CO_2 in a 30 mass percent monoethanolamine solution.CJChE.1995,73(1):140-147.
    [73]P.M.M.Blauwhoff,G.F.Versteeg,W.P.M.Van Swaaij.A study on the reaction between CO_2and alkanolamines in aqueous solutions.Chem.Eng.Sci.,1984,39(2):207-225.
    [74]David A.Glasscock,James E.Critchfield,Gary T.Rochelle.CO_2 Absorption/Desorption in mixture of Methyldiethanolamine with Monoethanolamine or Diethanolamine.Chem.Eng.Sci.,1991,46(11):2829-2845.
    [75]Little R.J.,van Swaaij W.P.M.,Versteeg G.F.Kinetics of Carbon dioxide with teriary amines in aqueous solution.AlChe.J.,1990,36(11):1633-1640.
    [76]H.Bosch,G.F.Versteeg,W.P,M.Van Swaaij.Gas-Liquid Mass Transfer with Parallel Reversible Reactions-Ⅲ.Absorption of CO_2 into Solutions of Blends of Amines.Chem.Eng.Sci.,1989,44(11):2745-2750.
    [77]David M.Austgen,Gary T.Rochelle,Chau Chyun Chen.Model of vapor-liquid equilibria for aqueous acid gas-alkanolamine systems.2,Representation of hydrogen sulfide and carbon dioxide solubility in aqueous MDEA and carbon dioxide solubility in aqueous mixtures of MDEA with MEA or DEA.Ind.Chem.Res.,1991,30(3):543-555.
    [78]A.Chakma.An Energy Efficient Mixed Solvent for The Separation of CO_2.Energy Conveys.Mgmt,1995,36(6-9):427-430.
    [79]Norio Arashi,Naoki Oda,Mutsuo Yamada,et al.Evaluation of Test Results of 1000m~3N/h Pilot Plant for CO_2 Absorption Using An Amine-Based Solution.Energy Conveys.Mgmt.,1997,38(1):63-68.
    [80]Danielle Bonenfant,Murielle Mimeault,Robert Hausler.Comparative Analysis of the Carbon Dioxide Absorption and Recuperation Capacities in Aqueous 2-(2-Aminoethylamino)ethanol(AEE)and Blends of Aqueous AEE and N-Methyldiethanolamine Solutions.Ind.Eng.Chem.Res.2005,44(10):3720-3725.
    [81]谭大志.溶液法富集CO_2的基础研究(硕士论文).大连:大连理工大学,2005.
    [82]Erdoean Alper.Reaction Mechanism and Kinetics of Aqueous Solutions of 2-Amino-2-methyl-1-propanoland Carbon Dioxide,Ind.Eng.Chem.Res.,1990.29(8):1725-1728.
    [83] G. F. Versteeg, J. A. M. Kuipers, F. P. H. Van Beckum. et al.Mass transfer with complex reversible chemical reactions-II. parallel reversible chemical reactions. Chem. Eng. Sci. 1990,45 (1):183-197.

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