Simultaneous absorption of SO2 and CO2 from flue gas using aqueous ammonia
QI Guojie, WANG Shujuan, GAO Jubao, LIU Jinzhao, ZHAO Bo, ZHUO Yuqun, CHEN Changhe
Beijing Key Laboratory for CO2 Utilization and Reduction Technology, Key Laboratory for Thermal Science and Power Engineering of the Ministry of Education, Department of Thermal Engineering, Tsinghua University, Beijing 100084, China
Abstract：Coal-fired power plants emit large quantities of SO2 and CO2, so more research is needed on SO2 and CO2 capture. Experimental tests were conducted in a wetted wall column system to analyze the simultaneous absorption of SO2 and CO2 using aqueous ammonia (weight percent, 0.2%-7%). The Aspen Plus RateSep model was then used to analyze the CO2 and SO2 mass transfer in the packed column to comprise the design of the ammonia based CO2 and SO2 absorption system. The experiments show that the SO2 selectivity absorption factor decreases as the CO2 volume concentration increases. The CO2 volume concentration (5%-20%) has little effect on the SO2 mass transfer and the SO2 absorption rate is always an order of magnitude higher than that of CO2. Increasing the SO2 mass concentration and reaction temperature has a negative effect on the CO2 absorption and the ammonia tends to selectively absorb the SO2. When the SO2 loading (mole concentration ratio between SO2 and NH3 in the aqueous ammonia solvent) increases from 0.1 to 0.4, the CO2 mass transfer rate significantly decreases. Increasing the ammonia mass concentration improves the absorption of both CO2 and SO2 and the predicted results are in good agreement with the experimental data. Thus, the packed column combined with an ammonia scrubber to reduce the ammonia slip and a resin exchange device used to control the SO2 loading can achieve simultaneous removal of CO2 and SO2.
齐国杰, 王淑娟, 高巨宝, 刘今朝, 赵博, 禚玉群, 陈昌和. 氨水溶液同时吸收烟气中SO2和CO2的实验及模拟[J]. 清华大学学报（自然科学版）, 2016, 56(8): 885-892.
QI Guojie, WANG Shujuan, GAO Jubao, LIU Jinzhao, ZHAO Bo, ZHUO Yuqun, CHEN Changhe. Simultaneous absorption of SO2 and CO2 from flue gas using aqueous ammonia. Journal of Tsinghua University(Science and Technology), 2016, 56(8): 885-892.
[1] 马广大.大气污染控制工程[M].北京:中国环境科学出版社,2002.MA Guangda.Air Pollution Control Engineering[M].Beijing:China Environmental Science Press,2002.(in Chinese)
[2] 白冰,李小春,刘延峰,等.中国CO2集中排放源调查及其分布特征[J].岩石力学与工程学报,2006,25(S1):2918-2923.BAI Bing,LI Xiaochun,LIU Yanfeng,et al.Preliminary study on CO2 industrial point sources and their distribution in China[J].Chinese Journal of Rock Mechanics and Engineering,2006,25(S1):2918-2923.(in Chinese)
[3] Shaw D.Cansolv CO2 capture:The value of integration[J].Energy Procedia,2009,1:237-246.
[4] GAO Jubao,WANG Shujuan,ZHOU Shan,et al.Corrosion and degradation performance of novel absorbent for CO2 capture in pilot-scale[J].Energy Procedia,2011,4:1534-1541.
[5] Sexton J A.Amine Oxidation in CO2 Capture Processes[D].Austin:University of Texas at Austin,2008.
[6] Closmanna F,Rochelle T G.Degradation of aqueous methyldiethanolamine by temperature and oxygen cycling[J].Energy Procedia,2011,4:23-28.
[7] 翁淑容.有机胺湿法脱硫实验研究[D].南京:南京理工大学,2007.WENG Shurong.Experimental Study on Wet Desulfurization using Amine[D].Nanjing:Nanjing University of Science,2007.(in Chinese)
[8] 翟林智,钟秦,王娟.可再生乙二胺湿法烟气脱硫实验研究[J].中国电机工程学报,2009,29(29):57-62.ZHAI Linzhi,ZHONG Qin,WANG Juan.Experimental study on the regenerable wet flue gas desulfurization with ethylenediamine[J].Proceedings of the CSEE,2009,29(29):57-62.(in Chinese)
[9] Mandal B P,Bandyopadhyay S S.Simultaneous absorption of CO2 and H2S into aqueous blends of 2-amino-2-methyl-1-propanol and diethanolamine[J].Chemical Engineering Science,2005,60:6438-6451.
[10] 张成芳.醇胺溶液吸收硫化氢和二氧化碳(二):同时吸收和吸收的选择性[J].石油与天然气化工,1984,13(6):10-19.ZHANG Chengfang.H2S and CO2 absorption using amine:Simultaneous absorption and selective absorption[J].Chemical Engineering of Oil and Gas,1984,13(6):10-19.(in Chinese)
[11] Pacheco M,Rochelle T G.Rate-based modeling of reactive absorption of CO2 and H2S intoaqueous methyldiethanolamine[J].Ind Eng Chem Res,1998,37:4107-4117.
[12] Park S,Park D,Oh K,et al.Simultaneous absorption of CO2 and SO2 into aqueous 2-amino-2-methy-1-propanol[J].Separation Science and Technology,2009,44(3):543-568.
[13] Choi W,Min B,Shon B,et al.Effect of ammonia on the absorption kinetics of carbon dioxide into aqueous 2-amino-2-methyl-1-propanol solutions[J].Ind Eng Chem Res,2009,48(8):4022-4029.
[14] 仇中柱,龚少林,郑超润,等.填料塔内氨水同时吸收SO2和CO2的试验研究[J].动力工程学报,2011,31(9):700-704.QIU Zhongzhu,GONG Shaolin,ZHENG Chaorun,et al.Simultaneous absorption of SO2 and CO2 by aqueous ammonia in a packed column[J].Journal of Chinese Society of Power Engineering,2011,31(9):700-704.(in Chinese)
[15] 刘芳,王淑娟,陈昌和,等.电厂烟气氨法脱碳技术研究进展[J].化工学报,2009,60(2):269-278.LIU Fang,WANG Shujuan,CHEN Changhe,et al.Research progress of CO2 capture by using ammonia from flue gas of power plant[J].Journal of the Chemical Industry and Engineering,2009,60(2):269-278.(in Chinese)
[16] 钟秦.燃煤烟气脱硫脱硝技术及工程实例[M].北京:化学工业出版社,2007.ZHONG Qin.Coal-fired Flue Gas Desulfurization and Denitrification Technology and Pilot Plant Demonstration[M].Beijing:Chemical Industry Press,2007.(in Chinese)
[17] 秦锋.氨水吸收二氧化碳的化学反应动力学与吸收热研究[D].北京:清华大学,2010.QIN Feng.Study on Kinetics and Heat of Absorption of CO2 in Aqueous Ammonia[D].Beijing:Tsinghua University,2010.(in Chinese)
[18] Resnik P K.Aqua ammonia process for simultaneous removal of CO2,SO2 and NOx[J].International Journal of Environmental Technology and Management,2004,4:89-104.
[19] 齐国杰,王淑娟,刘今朝,等.燃煤烟气中CO2对氨法脱碳的影响[J].化工学报,2012,63(7):2202-2209.QI Guojie,WANG Shujuan,LIU Jinzhao,et al.Impact of SO2 on CO2 capture in coal-fired flue gas using aqueous ammonia[J].Journal of the Chemical Industry and Engineering,2012,63(7):2202-2209.(in Chinese)
[20] Ebrahimi S,Picioreanu C,Kleerebezem R,et al.Rate-based modeling of SO2 absorption into aqueous NaHCO3/Na2CO3 solutions accompanied by the desorption of CO2[J].Chemical Engineering Science,2003,58:3589-3600.
[21] Liu J,Wang S,Zhao B,et al.Absorption of carbon dioxide in aqueous ammonia[J].Energy Procedia,2009,1:933-940.
[22] Yih S,Sun C.Simultaneous absorption of H2S and CO2 into di-isopropanolamine solution[J].The Canadian Journal of Chemical Engineering,1987,65(4):581-585.
[23] Zhang Y,Chen H,Chen C,et al.Rate-based process modeling study of CO2 capture withaqueous monoethanolamine solution[J].Ind Eng Chem Res,2009,48:9233-9246.
[24] Chen E.Carbon Dioxide Absorption into Piperazine Promoted Potassium Carbonate using Structured Packing[D].Austin:University of Texas at Austin,2007.
[25] Kozak F,Petig A,Morris E,et al.Chilled ammonia process for CO2 capture[J].Energy Procedia,2009,1:1419-1426.
[26] 高巨宝.胺法捕集燃煤电厂烟气中CO2的中试实验研究[D].北京:清华大学,2012.GAO Jubao.Pilot-scale Experimental Study on CO2 Capture using Amine-based Absorbent from Coal-fired Power Plants[D].Beijing:Tsinghua University,2012.(in Chinese)
2016, Vol. 56 
