陶瓷膜接触器在润湿模式下吸收SO_2的传质强化
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摘要
将平均孔径为100 nm的Al_2O_3陶瓷膜组装成膜接触器,以单乙醇胺(MEA)为吸收剂,在考察吸收剂浓度对膜吸收过程影响的基础上,深入比较了陶瓷膜在润湿和非润湿模式下脱除SO_2的传质性能.实验结果表明,当MEA浓度大于0.26 mol·L~(-1)时,润湿模式下SO_2的脱除率和传质系数均高于非润湿模式.根据膜理论和阻力串联模型建立了陶瓷膜吸收SO_2的传质方程,理论计算表明,润湿模式下膜相传质阻力因瞬间化学反应的存在大幅降低,润湿模式更适用于脱除烟气中低浓度的SO_2.本研究结果可为陶瓷膜接触器在膜吸收领域的工业化应用和进一步传质优化提供参考.
In this work, a study of removing acid gas via ceramic membrane contactor was carried out with monoethanolamine(MEA) used as absorbent. Two kinds of Al_2O_3 ceramic membrane with hydrophobic and hydrophilic properties were assembled to the membrane contactor and operated at wetted mode and non-wetted mode, respectively. On the basis of investigating the influence of absorbent concentration on the absorption process, the mass transfer performance of ceramic membrane absorbing SO_2 in the two modes was compared. The experiments showed that when the MEA concentration was higher than 0.26 mol·L~(-1), the removal efficiency and mass transfer coefficient of SO_2 in the wetted mode were higher than those in the non-wetted mode. The theoretical calculation indicated that the membrane mass transfer resistance in the wetting mode was greatly decreased because of the transient chemical reaction, and the wetting mode is more suitable for the removal of the low concentration of SO_2 in the flue gas. The results of this work can provide reference for industrial application and further mass transfer optimization of ceramic membrane contactors in the field of membrane gas absorption.
In this work, a study of removing acid gas via ceramic membrane contactor was carried out with monoethanolamine(MEA) used as absorbent. Two kinds of Al_2O_3 ceramic membrane with hydrophobic and hydrophilic properties were assembled to the membrane contactor and operated at wetted mode and non-wetted mode, respectively. On the basis of investigating the influence of absorbent concentration on the absorption process, the mass transfer performance of ceramic membrane absorbing SO_2 in the two modes was compared. The experiments showed that when the MEA concentration was higher than 0.26 mol·L~(-1), the removal efficiency and mass transfer coefficient of SO_2 in the wetted mode were higher than those in the non-wetted mode. The theoretical calculation indicated that the membrane mass transfer resistance in the wetting mode was greatly decreased because of the transient chemical reaction, and the wetting mode is more suitable for the removal of the low concentration of SO_2 in the flue gas. The results of this work can provide reference for industrial application and further mass transfer optimization of ceramic membrane contactors in the field of membrane gas absorption.
引文
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Chen X F,Gao X Y,Fu K Y,et al.2018.Tubular hydrophobic ceramic membrane with asymmetric structure for water desalination via vacuum membrane distillation process[J].Desalination,443:212-220
Dai Z D,Usman M,Hillestad M,et al.2016.Modelling of a tubular membrane contactor for pre-combustion CO2 capture using ionic liquids:Influence of the membrane configuration,absorbent properties and operation parameters[J].Green Energy& Enviroment,1:266-275
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丁兆阳,韩治洋,石文荣,等.2018.快速变压吸附制氧动态传质系数模拟分析[J].化工学报,69(2):759-768
Faiz R,Al-Marzouqi M.2009.Mathematical modeling for the simultaneous absorption of CO2 and H2S using MEA in hollow fiber membrane contactors[J].Journal of Membrane Science,342(1/2):269-278
Gao J B,Wang S J,Zhao B,et al.2011.Pilot-scale experimental study on the CO2 capture process with existing of SO2:Degradation,reaction rate,and mass transfer[J].Energy & Fuels,25(12):5802-5809
Gao N W,Li M,Jing W H,et al.2011.Improving the filtration performance of ZrO2 membrane in non-polar organic solvents by surface hydrophobic modification[J].Journal of Membrane Science,375(1/2):276-283
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李志娟,曹利,黄学敏.2016.膜法氨水吸收脱除烟气中CO2的研究[J].环境科学学报,36(3):1050-1056
Lee H J,Magnone E,Park J H.2015.Preparation,characterization and laboratory-scale application of modified hydrophobic aluminum oxide hollow fiber membrane for CO2 capture using H2O as low-cost absorbent[J].Journal of Membrane Science,494:143-153
Luis P,Garea A,Irabien A.2010.Modelling of a hollow fibre ceramic contactor for SO2 absorption[J].Separation and Purification Technology,72:174-179
Lv Y X,Yu X H,Jia J J,et al.2012.Fabrication and characterization of superhydrophobic polypropylene hollow fiber membranes for carbon dioxide absorption[J].Applied Energy,90(1):167-174
Mansourizadeh A,Ismail A F.2009.Hollow fiber gas-liquid membrane contactors for acid gas capture:a review[J].J Hazard Mater,171(1/3):38-53
Mathias L,Klaudia G N,Rudiger S.2018.Enzymatic reactive absorption of CO2 in MDEA by means of an innovative biocatalyst delivery system[J].Chemical Engineering Journal,334:1195-1205
Mohammad M G,Amir H M.2014.Rigorous modeling of CO2 equilibrium absorption in MEA,DEA,and TEA aqueous solutions[J].Journal of Natural Gas Science and Engineering,18:39-46
Mosadegh-Sedghi S,Rodrigue D,Brisson J,et al.2014.Wetting phenomenon in membrane contactors-Causes and prevention[J].Journal of Membrane Science,452:332-353
Qi G J,Wang S J,Lu W Y,et al.2015.Vapor-liquid equilibrium of CO2 in NH3-CO2-SO2-H2O system[J].Fluid Phase Equilibria,386:47-55
Rangwala H A.1996.Absorption of carbon dioxide into aqueous solutions using hollow fiber membrane contactors[J].Journal of Membrane Science,112(2):229-240
Rongwong W,Fan C,Liang Z W,et al.2015.Investigation of the effects of operating parameters on the local mass transfer coefficient and membrane wetting in a membrane gas absorption process[J].Journal of Membrane Science,490:236-246
Rongwong W,Jiraratananon R,Atchariyawut S.2009.Experimental study on membrane wetting in gas-liquid membrane contacting process for CO2 absorption by single and mixed absorbents[J].Separation and Purification Technology,69(1):118-125
Sreedhar I,Nahar T,Venugopal A,et al.2017.Carbon capture by absorption-Path covered and ahead[J].Renewable and Sustainable Energy Reviews,76:1080-1107
Wu X,Zhao B,Wang L,et al.2016.Hydrophobic PVDF/graphene hybrid membrane for CO2 absorption in membrane contactor[J].Journal of Membrane Science,520:120-129
徐建新,张洪起,刘继东,等2013.电解质NRTL模型的研究进展及应用[J].化工进展,32(9):2023-2029
Yan S P,Fang M X,Zhang W F,et al.2007.Experimental study on the separation of CO2 from flue gas using hollow fiber membrane contactors without wetting[J].Fuel Processing Technology,88(5):501-511
Yu X H,An L,Yang J,et al.2015.CO2 capture using a superhydrophobic ceramic membrane contactor[J].Journal of Membrane Science,496:1-12
Zhang Q,Cussler E L.1985a.Microporous hollow fibers for gas-absorption.1.Mass-transfer in the liquid[J].Journal of Membrane Science,23(3):321-332
Zhang Q,Cussler E L.1985b.Microporous hollow fibers for gas-absorption.2.Mass-transfer in the liquid[J].Journal of Membrane Science,23(3):333-345
Zhang T,Yu Y,Zhang Z.2018.An interactive chemical enhancement of CO2 capture in the MEA/PZ/AMP/DEA binary solutions[J].International Journal of Greenhouse Gas Control,74:119-129
Zou D,Qiu M H,Chen X F,et al.2017.One-step preparation of high-performance bilayer α-alumina ultrafiltration membranes via co-sintering process[J].Journal of Membrane Science,524:141-150
Chen X F,Gao X Y,Fu K Y,et al.2018.Tubular hydrophobic ceramic membrane with asymmetric structure for water desalination via vacuum membrane distillation process[J].Desalination,443:212-220
Dai Z D,Usman M,Hillestad M,et al.2016.Modelling of a tubular membrane contactor for pre-combustion CO2 capture using ionic liquids:Influence of the membrane configuration,absorbent properties and operation parameters[J].Green Energy& Enviroment,1:266-275
Demyanovich R,Lynn S.1987.Vapor-liquid equilibria of sulfur dioxide in polar organic solvents[J].Ind Eng Chem Res,26(3):548-555
丁兆阳,韩治洋,石文荣,等.2018.快速变压吸附制氧动态传质系数模拟分析[J].化工学报,69(2):759-768
Faiz R,Al-Marzouqi M.2009.Mathematical modeling for the simultaneous absorption of CO2 and H2S using MEA in hollow fiber membrane contactors[J].Journal of Membrane Science,342(1/2):269-278
Gao J B,Wang S J,Zhao B,et al.2011.Pilot-scale experimental study on the CO2 capture process with existing of SO2:Degradation,reaction rate,and mass transfer[J].Energy & Fuels,25(12):5802-5809
Gao N W,Li M,Jing W H,et al.2011.Improving the filtration performance of ZrO2 membrane in non-polar organic solvents by surface hydrophobic modification[J].Journal of Membrane Science,375(1/2):276-283
Gilliland E R.1934.Diffusion coefficients in gaseous systems[J].Industrial & Engineering Chemistry,26(6):681-685
Hashemifard S A,Mstsuura T,Ismail A F,et al.2015.Characterization of partial pore wetting in hollow fiber gas absorption membrane contactors:An EDX analysis approach[J].Chemical Engineering Journal,281:970-980
韩士贤,高兴银,符开云,等.2017.疏水性单管陶瓷膜接触器在SO2吸收中的应用[J].化工学报,68(6):2415-2422
李志娟,曹利,黄学敏.2016.膜法氨水吸收脱除烟气中CO2的研究[J].环境科学学报,36(3):1050-1056
Lee H J,Magnone E,Park J H.2015.Preparation,characterization and laboratory-scale application of modified hydrophobic aluminum oxide hollow fiber membrane for CO2 capture using H2O as low-cost absorbent[J].Journal of Membrane Science,494:143-153
Luis P,Garea A,Irabien A.2010.Modelling of a hollow fibre ceramic contactor for SO2 absorption[J].Separation and Purification Technology,72:174-179
Lv Y X,Yu X H,Jia J J,et al.2012.Fabrication and characterization of superhydrophobic polypropylene hollow fiber membranes for carbon dioxide absorption[J].Applied Energy,90(1):167-174
Mansourizadeh A,Ismail A F.2009.Hollow fiber gas-liquid membrane contactors for acid gas capture:a review[J].J Hazard Mater,171(1/3):38-53
Mathias L,Klaudia G N,Rudiger S.2018.Enzymatic reactive absorption of CO2 in MDEA by means of an innovative biocatalyst delivery system[J].Chemical Engineering Journal,334:1195-1205
Mohammad M G,Amir H M.2014.Rigorous modeling of CO2 equilibrium absorption in MEA,DEA,and TEA aqueous solutions[J].Journal of Natural Gas Science and Engineering,18:39-46
Mosadegh-Sedghi S,Rodrigue D,Brisson J,et al.2014.Wetting phenomenon in membrane contactors-Causes and prevention[J].Journal of Membrane Science,452:332-353
Qi G J,Wang S J,Lu W Y,et al.2015.Vapor-liquid equilibrium of CO2 in NH3-CO2-SO2-H2O system[J].Fluid Phase Equilibria,386:47-55
Rangwala H A.1996.Absorption of carbon dioxide into aqueous solutions using hollow fiber membrane contactors[J].Journal of Membrane Science,112(2):229-240
Rongwong W,Fan C,Liang Z W,et al.2015.Investigation of the effects of operating parameters on the local mass transfer coefficient and membrane wetting in a membrane gas absorption process[J].Journal of Membrane Science,490:236-246
Rongwong W,Jiraratananon R,Atchariyawut S.2009.Experimental study on membrane wetting in gas-liquid membrane contacting process for CO2 absorption by single and mixed absorbents[J].Separation and Purification Technology,69(1):118-125
Sreedhar I,Nahar T,Venugopal A,et al.2017.Carbon capture by absorption-Path covered and ahead[J].Renewable and Sustainable Energy Reviews,76:1080-1107
Wu X,Zhao B,Wang L,et al.2016.Hydrophobic PVDF/graphene hybrid membrane for CO2 absorption in membrane contactor[J].Journal of Membrane Science,520:120-129
徐建新,张洪起,刘继东,等2013.电解质NRTL模型的研究进展及应用[J].化工进展,32(9):2023-2029
Yan S P,Fang M X,Zhang W F,et al.2007.Experimental study on the separation of CO2 from flue gas using hollow fiber membrane contactors without wetting[J].Fuel Processing Technology,88(5):501-511
Yu X H,An L,Yang J,et al.2015.CO2 capture using a superhydrophobic ceramic membrane contactor[J].Journal of Membrane Science,496:1-12
Zhang Q,Cussler E L.1985a.Microporous hollow fibers for gas-absorption.1.Mass-transfer in the liquid[J].Journal of Membrane Science,23(3):321-332
Zhang Q,Cussler E L.1985b.Microporous hollow fibers for gas-absorption.2.Mass-transfer in the liquid[J].Journal of Membrane Science,23(3):333-345
Zhang T,Yu Y,Zhang Z.2018.An interactive chemical enhancement of CO2 capture in the MEA/PZ/AMP/DEA binary solutions[J].International Journal of Greenhouse Gas Control,74:119-129
Zou D,Qiu M H,Chen X F,et al.2017.One-step preparation of high-performance bilayer α-alumina ultrafiltration membranes via co-sintering process[J].Journal of Membrane Science,524:141-150
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