磁场对氨水吸收烟气中CO_2的促进作用
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摘要
开发了一种新型磁场辅助氨法烟气脱碳技术。含碳烟气通入混有磁性颗粒的氨水溶液,在外加磁场的作用下发生脱碳反应。对该技术的运行特性开展了实验研究。结果表明,外加8 m T恒稳磁场,2 g·L~(-1)纳米级Fe_3O_4颗粒,氨水的CO_2脱除效率比不添加磁场和颗粒时最多可提高8.8%。外加磁场可以有效提高低浓度氨水的CO_2脱除效率。在模拟烟气流量增加时,外加磁场能有效减缓CO_2脱除效率下降的趋势。同时,外加磁场使得CO_2脱除效率曲线向低温方向移动5℃,有助于提高低温条件下的CO_2脱除效率。磁场可提高气液接触效率、降低相间传质阻力、增强氨水反应活性,从而提高氨水吸收CO_2性能。
A novel ammonia-based CO_2 capture process was proposed in the paper. The process uses magnetically gas-solid-liquid bed as the reactor in which the ferromagnetic particles suspend in aqueous ammonia solutions under the influence of external magnetic field(EMF). A continuous of CO_2 passed through the reactor was absorbed by aqueous ammonia. Experiments in a laboratory-scale apparatus were carried out to investigate the roles of EMF. The results showed that the highest CO_2 absorption efficiency with 8 m T EMF and 2 g·L~(-1)nano-magnetic particles reached 94.3%, more than 8.8% compared to that without EMF and nanoparticles. CO_2 absorption efficiency with EMF and nanoparticles increased significantly under the conditions of low concentration aqueous ammonia(5%—8%), large flux of simulated flue gas(3.5 L·min~(-1)) and low absorption temperature(22—36℃). The enhancement of CO_2 absorption under the influence of EMF and nanoparticles should be attributed to good gas-liquid contact, large mass transfer coefficient and high reactivity of aqueous ammonia.
A novel ammonia-based CO_2 capture process was proposed in the paper. The process uses magnetically gas-solid-liquid bed as the reactor in which the ferromagnetic particles suspend in aqueous ammonia solutions under the influence of external magnetic field(EMF). A continuous of CO_2 passed through the reactor was absorbed by aqueous ammonia. Experiments in a laboratory-scale apparatus were carried out to investigate the roles of EMF. The results showed that the highest CO_2 absorption efficiency with 8 m T EMF and 2 g·L~(-1)nano-magnetic particles reached 94.3%, more than 8.8% compared to that without EMF and nanoparticles. CO_2 absorption efficiency with EMF and nanoparticles increased significantly under the conditions of low concentration aqueous ammonia(5%—8%), large flux of simulated flue gas(3.5 L·min~(-1)) and low absorption temperature(22—36℃). The enhancement of CO_2 absorption under the influence of EMF and nanoparticles should be attributed to good gas-liquid contact, large mass transfer coefficient and high reactivity of aqueous ammonia.
引文
[1]朱德臣.燃煤烟气CO2化学吸收技术研究[D].杭州:浙江大学,2011.ZHU D C.Chemical absorption of CO2 from flue gas[D].Hangzhou:Zhejiang University,2011.
[2]陈健,罗伟亮,李晗.有机胺吸收二氧化碳的热力学和动力学研究进展[J].化工学报,2014,65(1):12-21.CHEN J,LUO W L,LI H.Advances in thermodynamics and kinetics of organic amine to absorb carbon dioxide[J].CIESC Journal,2014,65(1):12-21.
[3]SHAKERIAN F,KIM K H,SZULEJKO J E,et al.A comparative review between amines and ammonia as sorptive media for post-combustion CO2 capture[J].Applied Energy,2015,148:10-22.
[4]BAI H,YEH A C.Removal of CO2 greenhouse gas by ammonia scrubbing[J].Industrial&Engineering Chemistry Research,1997,36(6):2490-2493.
[5]YEH A C,BAI H.Comparison of ammonia and monoethanolamine solvents to reduce CO2 greenhouse gas emissions[J].Science of the Total Environment,1999,228(2):121-133.
[6]KIM Y J,YOU J K,HONG W H,et al.Characteristics of CO2absorption into aqueous ammonia[J].Separation Science and Technology,2008,43(4):766-777.
[7]QIN F,WANG S J,HARTONO A,et al.Kinetics of CO2 absorption in aqueous ammonia solution[J].International Journal of Greenhouse Gas Control,2010,4(5):729-738.
[8]PARK S Y,YI K B,CHANG H K,et al.Selection of optimal operating conditions for a continuous CO2-capture process using an aqueous ammonia solution[J].Energy&Fuels,2010,24(6):3704-3709.
[9]VERSTEEG P,RUBIN E S.A technical and economic assessment of ammonia-based post-combustion CO2 capture at coal-fired power plants[J].International Journal of Greenhouse Gas Control,2011,5(6):1596-1605.
[10]ZHANG M K,GUO Y C.Rate based modeling of absorption and regeneration for CO2 capture by aqueous ammonia solution[J].Applied Energy,2013,111(4):142-152.
[11]DANIEL S,MATTEO G,MARCO M.Formation of solids in ammonia-based CO2 capture processes-identification of criticalities through thermodynamic analysis of the CO2-NH3-H2O system[J].Chemical Engineering Science,2015,133:170-180.
[12]QUE H L,CHEN C C.Thermodynamic modeling of the NH3-CO2-H2O system with electrolyte NRTL model[J].Industrial&Engineering Chemistry Research,2011,50(19):11406-11421.
[13]BAK C U,ASIF M,KIM W S.Experimental study on CO2 capture by chilled ammonia process[J].Chemical Engineering Journal,2014,265(5):1-8.
[14]YU J,WANG S.Development of a novel process for aqueous ammonia based CO2 capture[J].International Journal of Greenhouse Gas Control,2015,39:129-138.
[15]马双忱,陈公达,温佳琪,等.氨法脱碳过程中氨逃逸规律及其抑制[J].化工学报,2016,67(5):2064-2069.MA S C,CHEN G D,WEN J Q,et al.Ammonia escape and its prevention in CO2 absorption process using ammonia solution[J].CIESC Journal,2016,67(5):2064-2069.
[16]张宇,高建民,何明月,等.两种强化低碳化度氨水结晶的新型氨法脱碳工艺[J].化工学报,2015,66(6):2123-1230.ZHANG Y,GAO J M,HE M Y,et al.Two kinds of new carbon capture technology by ammonia based on reinforced crystallization[J].CIESC Journal,2015,66(6):2123-1230.
[17]冷浩,高建民,张宇,等.强化结晶氨法脱碳实验研究[J].化工学报,2016,67(6):2440-2448.LENG H,GAO J M,ZHANG Y,et al.Carbon capture by ammonia with reinforced crystallization[J].CIESC Journal,2016,67(6):2440-2448.
[18]彭远昌,赵兵涛,李蕾蕾,等.鼓泡式反应器高径比对氨法烟气脱碳性能的影响[J].化工环保,2013,33(3):206-209.PENG Y C,ZHAO B T,LI L L,et al.Effect of bubble reactor height to diameter ratio of ammonia flue gas decarbonization performance[J].Environmental Protection of Chemical Industry,2013,33(3):206-209.
[19]马双忱,孙云雪,赵毅,等.氨水捕集模拟烟气中二氧化碳的实验与理论研究[J].化学学报,2011,69(12):1469-1474.MA S C,SUN Y X,ZHAO Y,et al.Experimental and theoretical studies simulated flue gas ammonia trapping carbon dioxide[J].Acta Chemical,2011,69(12):1469-1474.
[20]刘芳.再生氨法脱除燃煤电厂烟气中二氧化碳的实验研究[D].北京:清华大学,2009.LIU F.Experimental study of regeneration ammonia removal of carbon dioxide in the flue gas of coal-fired power plant[D].Beijing:Tsinghua University,2009.
[21]RESNIK K P,PENNLINE H W.Study of an ammonia-based wet scrubbing process in a continuous flow system[J].Fuel,2013,105(1):184-191.
[22]MA S C,ZANG B,SONG H H,et al.Research on mass transfer of CO2 absorption using ammonia solution in spray tower[J].International Journal of Heat&Mass Transfer,2013,67(12):696-703.
[23]KONG D J,ZHANG Y F,LI N,et al.Experimental investigation on gas-liquid flow,heat and mass transfer characteristics in a dual-contact-flow absorption tower[J].Chemical Engineering Research&Design,2014,92(1):13-24.
[24]ZHAO B T,SU Y X,TAO W W.Mass transfer performance of CO2capture in rotating packed bed:dimensionless modeling and intelligent prediction[J].Applied Energy,2014,136:132-142.
[25]LI J L,CHEN B H.Review of CO2 absorption using chemical solvents in hollow fiber membrane contactors[J].Separation&Purification Technology,2005,41(2):109-122.
[26]YANG N,YU H,XU D Y,et al.Amino acids/NH3 mixtures for CO2capture:effect of neutralization methods on CO2 mass transfer and NH3 vapour loss[J].Energy Procedia,2014,63:773-780.
[27]LI L,CONWANE W,PUXTY G,et al.The effect of piperazine(PZ)on CO2 absorption kinetics into aqueous ammonia solutions at 25.0℃[J].International Journal of Greenhouse Gas Control,2015,36:135-143.
[28]ZHI H L,LEE K T,BHATIA S,et al.Post-combustion carbon dioxide capture:evolution towards utilization of nanomaterials[J].Renewable&Sustainable Energy Reviews,2012,16(5):2599-2609.
[29]JUNG J Y,LEE J W,KANG Y T.CO2 absorption characteristics of nanoparticle suspensions in methanol[J].Journal of Mechanical Science and Technology,2012,26(8):2285-2290.
[30]JIANG J Z,ZHAO B,CAO M,et al.Chemical absorption kinetics in MEA solution with nano-particles[J].Energy Procedia,2013,37:518-524.
[31]YANG L,DU K,NIU X F,et al.Experimental study on enhancement of ammonia-water falling film absorption by adding nano-particles[J].International Journal of Refrigeration,2011,34(3):640-647.
[32]ZENG P,ZHOU T,YANG J S.Behavior of mixtures of nano-particles in magnetically assisted fluidized bed[J].Chemical Engineering and Processing,2008,47:101-108.
[33]宗保宁,慕旭宏,孟祥堃,等.镍基非晶态合金加氢催化剂与磁稳定床反应器的开发与工业应用[J].化工进展,2002,21(8):536-539.ZONG B N,MU X H,MENG X K,et al.Amorphous skeletal nickel-based alloy catalyst and magnetically stabilized bed reactor[J].Chemical Industry&Engineering Progress,2002,21(8):536-539.
[34]LIU Y A,KEITY H,COLBERG R.Fundamental and practical developments of magnetofluidized beds[J].Powder Technology,1991,64(1/2):3-41.
[35]ZHANG Q,GUI K T,WANG X B.Effects of magnetic fields on improving mass transfer in flue gas desulfurization using a fluidized bed[J].Heat and Mass Transfer,2016,52:331-336.
[36]姚桂焕,陆芳,王芳,等.铁基磁流化床SCR烟气脱硝的磁场效应[J].工程热物理学报,2009,31:439-442.YAO G H,LU F,WANG F,et al.Reaction mechanism of flue gas desulfurization magnetically fluidized bed strengthen iron-based magnetic field effect fluidized-bed selective catalytic reduction flue gas denitrification[J].Journal of Engineering Thermophysics,2009,31:439-442.
[37]张春,武卫东,李增扬,等.磁场及纳米磁性流体强化氨水鼓泡吸收实验研究[J].磁性材料及器件,2014,45(3):21-24.ZHANG C,WU W D,LI Z Y,et al.Experimental study of ammonia bubble absorption of magnetic field and magnetic nanoparticles hydroenhancement[J].Journal of Magnetic Materials and Devices,2014,45(3):21-24.
[38]武卫东,庞常伟,盛伟,等.单体Ag纳米流体强化氨水鼓泡吸收特性[J].化工学报,2010,61(5):1112-1117.WU W D,PANG C W,SHENG W.Enhancement effects of Ag nanoparticles on ammonia bubble absorption[J].CIESC Journal,2010,61(5):1112-1117.
[39]齐国杰.氨水溶液联合脱除二氧化碳和二氧化硫的研究[D].北京:清华大学,2013.QI G J.Ammonia-based capture of CO2 and SO2 from flue gas[D].Beijing:Tsinghua University,2013.
[40]牛振祺,郭印诚,林文漪.MEA,Na OH与氨水喷雾捕集CO2性能[J].清华大学学报(自然科学版),2010,(7):1130-1134.NIU Z Q,GUO Y C,LIN W Y.MEA,Na OH and ammonia spray CO2capture performance[J].Journal of Tsinghua University(Science and Technology Edition),2010,(7):1130-1134.
[2]陈健,罗伟亮,李晗.有机胺吸收二氧化碳的热力学和动力学研究进展[J].化工学报,2014,65(1):12-21.CHEN J,LUO W L,LI H.Advances in thermodynamics and kinetics of organic amine to absorb carbon dioxide[J].CIESC Journal,2014,65(1):12-21.
[3]SHAKERIAN F,KIM K H,SZULEJKO J E,et al.A comparative review between amines and ammonia as sorptive media for post-combustion CO2 capture[J].Applied Energy,2015,148:10-22.
[4]BAI H,YEH A C.Removal of CO2 greenhouse gas by ammonia scrubbing[J].Industrial&Engineering Chemistry Research,1997,36(6):2490-2493.
[5]YEH A C,BAI H.Comparison of ammonia and monoethanolamine solvents to reduce CO2 greenhouse gas emissions[J].Science of the Total Environment,1999,228(2):121-133.
[6]KIM Y J,YOU J K,HONG W H,et al.Characteristics of CO2absorption into aqueous ammonia[J].Separation Science and Technology,2008,43(4):766-777.
[7]QIN F,WANG S J,HARTONO A,et al.Kinetics of CO2 absorption in aqueous ammonia solution[J].International Journal of Greenhouse Gas Control,2010,4(5):729-738.
[8]PARK S Y,YI K B,CHANG H K,et al.Selection of optimal operating conditions for a continuous CO2-capture process using an aqueous ammonia solution[J].Energy&Fuels,2010,24(6):3704-3709.
[9]VERSTEEG P,RUBIN E S.A technical and economic assessment of ammonia-based post-combustion CO2 capture at coal-fired power plants[J].International Journal of Greenhouse Gas Control,2011,5(6):1596-1605.
[10]ZHANG M K,GUO Y C.Rate based modeling of absorption and regeneration for CO2 capture by aqueous ammonia solution[J].Applied Energy,2013,111(4):142-152.
[11]DANIEL S,MATTEO G,MARCO M.Formation of solids in ammonia-based CO2 capture processes-identification of criticalities through thermodynamic analysis of the CO2-NH3-H2O system[J].Chemical Engineering Science,2015,133:170-180.
[12]QUE H L,CHEN C C.Thermodynamic modeling of the NH3-CO2-H2O system with electrolyte NRTL model[J].Industrial&Engineering Chemistry Research,2011,50(19):11406-11421.
[13]BAK C U,ASIF M,KIM W S.Experimental study on CO2 capture by chilled ammonia process[J].Chemical Engineering Journal,2014,265(5):1-8.
[14]YU J,WANG S.Development of a novel process for aqueous ammonia based CO2 capture[J].International Journal of Greenhouse Gas Control,2015,39:129-138.
[15]马双忱,陈公达,温佳琪,等.氨法脱碳过程中氨逃逸规律及其抑制[J].化工学报,2016,67(5):2064-2069.MA S C,CHEN G D,WEN J Q,et al.Ammonia escape and its prevention in CO2 absorption process using ammonia solution[J].CIESC Journal,2016,67(5):2064-2069.
[16]张宇,高建民,何明月,等.两种强化低碳化度氨水结晶的新型氨法脱碳工艺[J].化工学报,2015,66(6):2123-1230.ZHANG Y,GAO J M,HE M Y,et al.Two kinds of new carbon capture technology by ammonia based on reinforced crystallization[J].CIESC Journal,2015,66(6):2123-1230.
[17]冷浩,高建民,张宇,等.强化结晶氨法脱碳实验研究[J].化工学报,2016,67(6):2440-2448.LENG H,GAO J M,ZHANG Y,et al.Carbon capture by ammonia with reinforced crystallization[J].CIESC Journal,2016,67(6):2440-2448.
[18]彭远昌,赵兵涛,李蕾蕾,等.鼓泡式反应器高径比对氨法烟气脱碳性能的影响[J].化工环保,2013,33(3):206-209.PENG Y C,ZHAO B T,LI L L,et al.Effect of bubble reactor height to diameter ratio of ammonia flue gas decarbonization performance[J].Environmental Protection of Chemical Industry,2013,33(3):206-209.
[19]马双忱,孙云雪,赵毅,等.氨水捕集模拟烟气中二氧化碳的实验与理论研究[J].化学学报,2011,69(12):1469-1474.MA S C,SUN Y X,ZHAO Y,et al.Experimental and theoretical studies simulated flue gas ammonia trapping carbon dioxide[J].Acta Chemical,2011,69(12):1469-1474.
[20]刘芳.再生氨法脱除燃煤电厂烟气中二氧化碳的实验研究[D].北京:清华大学,2009.LIU F.Experimental study of regeneration ammonia removal of carbon dioxide in the flue gas of coal-fired power plant[D].Beijing:Tsinghua University,2009.
[21]RESNIK K P,PENNLINE H W.Study of an ammonia-based wet scrubbing process in a continuous flow system[J].Fuel,2013,105(1):184-191.
[22]MA S C,ZANG B,SONG H H,et al.Research on mass transfer of CO2 absorption using ammonia solution in spray tower[J].International Journal of Heat&Mass Transfer,2013,67(12):696-703.
[23]KONG D J,ZHANG Y F,LI N,et al.Experimental investigation on gas-liquid flow,heat and mass transfer characteristics in a dual-contact-flow absorption tower[J].Chemical Engineering Research&Design,2014,92(1):13-24.
[24]ZHAO B T,SU Y X,TAO W W.Mass transfer performance of CO2capture in rotating packed bed:dimensionless modeling and intelligent prediction[J].Applied Energy,2014,136:132-142.
[25]LI J L,CHEN B H.Review of CO2 absorption using chemical solvents in hollow fiber membrane contactors[J].Separation&Purification Technology,2005,41(2):109-122.
[26]YANG N,YU H,XU D Y,et al.Amino acids/NH3 mixtures for CO2capture:effect of neutralization methods on CO2 mass transfer and NH3 vapour loss[J].Energy Procedia,2014,63:773-780.
[27]LI L,CONWANE W,PUXTY G,et al.The effect of piperazine(PZ)on CO2 absorption kinetics into aqueous ammonia solutions at 25.0℃[J].International Journal of Greenhouse Gas Control,2015,36:135-143.
[28]ZHI H L,LEE K T,BHATIA S,et al.Post-combustion carbon dioxide capture:evolution towards utilization of nanomaterials[J].Renewable&Sustainable Energy Reviews,2012,16(5):2599-2609.
[29]JUNG J Y,LEE J W,KANG Y T.CO2 absorption characteristics of nanoparticle suspensions in methanol[J].Journal of Mechanical Science and Technology,2012,26(8):2285-2290.
[30]JIANG J Z,ZHAO B,CAO M,et al.Chemical absorption kinetics in MEA solution with nano-particles[J].Energy Procedia,2013,37:518-524.
[31]YANG L,DU K,NIU X F,et al.Experimental study on enhancement of ammonia-water falling film absorption by adding nano-particles[J].International Journal of Refrigeration,2011,34(3):640-647.
[32]ZENG P,ZHOU T,YANG J S.Behavior of mixtures of nano-particles in magnetically assisted fluidized bed[J].Chemical Engineering and Processing,2008,47:101-108.
[33]宗保宁,慕旭宏,孟祥堃,等.镍基非晶态合金加氢催化剂与磁稳定床反应器的开发与工业应用[J].化工进展,2002,21(8):536-539.ZONG B N,MU X H,MENG X K,et al.Amorphous skeletal nickel-based alloy catalyst and magnetically stabilized bed reactor[J].Chemical Industry&Engineering Progress,2002,21(8):536-539.
[34]LIU Y A,KEITY H,COLBERG R.Fundamental and practical developments of magnetofluidized beds[J].Powder Technology,1991,64(1/2):3-41.
[35]ZHANG Q,GUI K T,WANG X B.Effects of magnetic fields on improving mass transfer in flue gas desulfurization using a fluidized bed[J].Heat and Mass Transfer,2016,52:331-336.
[36]姚桂焕,陆芳,王芳,等.铁基磁流化床SCR烟气脱硝的磁场效应[J].工程热物理学报,2009,31:439-442.YAO G H,LU F,WANG F,et al.Reaction mechanism of flue gas desulfurization magnetically fluidized bed strengthen iron-based magnetic field effect fluidized-bed selective catalytic reduction flue gas denitrification[J].Journal of Engineering Thermophysics,2009,31:439-442.
[37]张春,武卫东,李增扬,等.磁场及纳米磁性流体强化氨水鼓泡吸收实验研究[J].磁性材料及器件,2014,45(3):21-24.ZHANG C,WU W D,LI Z Y,et al.Experimental study of ammonia bubble absorption of magnetic field and magnetic nanoparticles hydroenhancement[J].Journal of Magnetic Materials and Devices,2014,45(3):21-24.
[38]武卫东,庞常伟,盛伟,等.单体Ag纳米流体强化氨水鼓泡吸收特性[J].化工学报,2010,61(5):1112-1117.WU W D,PANG C W,SHENG W.Enhancement effects of Ag nanoparticles on ammonia bubble absorption[J].CIESC Journal,2010,61(5):1112-1117.
[39]齐国杰.氨水溶液联合脱除二氧化碳和二氧化硫的研究[D].北京:清华大学,2013.QI G J.Ammonia-based capture of CO2 and SO2 from flue gas[D].Beijing:Tsinghua University,2013.
[40]牛振祺,郭印诚,林文漪.MEA,Na OH与氨水喷雾捕集CO2性能[J].清华大学学报(自然科学版),2010,(7):1130-1134.NIU Z Q,GUO Y C,LIN W Y.MEA,Na OH and ammonia spray CO2capture performance[J].Journal of Tsinghua University(Science and Technology Edition),2010,(7):1130-1134.