用于膜接触器脱硫的PVDF/GO - IM膜制备与性能研究
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摘要
化石燃料燃烧和汽车尾气为PM2.5的重要来源,其中SO_2为PM2.5的重要组成部分,膜接触器在脱除SO_2领域具有良好的应用前景.本研究通过沉淀聚合法制备了氨基化氧化石墨烯(GO-IM),并填充到聚偏氟乙烯(PVDF)中,通过浸没沉淀相转化法制备了氨基化氧化石墨烯填充膜,对膜形貌、孔隙率、接触角和机械强度等进行表征,并评价其脱硫性能;此外,研究了不同GO-IM填充量的PVDF/GO-IM膜的渗透性能.结果表明,膜壁上的GO-IM可促进SO_2的传递,提高了SO_2气体的吸收通量,GO-IM上丰富的氨基提高了与PVDF界面的相容性.当GO-IM与PVDF质量比为3%、测试温度为20℃、进料气压力为0.10 MPa时,膜的SO_2吸收通量可达6.51×10~(-4) mol/(m~2·s),表明PVDF/GO-IM膜接触器在烟道气脱硫领域具有良好的应用前景.
Fossil fuel combustion and automobile exhaust are important sources of PM2.5, and SO_2 is an important component of PM2.5. Membrane contactors show excellent promising in the field of SO_2 removal. In this study, aminated graphene oxide(GO-IM) was synthetized by precipitation polymerization, and then was incorporated into polyvinylidene fluoride(PVDF) to fabricate aminated graphene oxide loaded membrane by immersion precipitation phase transformation. The morphology, porosity, contact angle and mechanical strength of membranes were characterized and the desulfurization performance of membranes was evaluated. In addition, the permeability of PVDF/GO-IM porous membranes with different GO-IM loadings was investigated. The results showed that the aminated graphene oxide on the porous membrane wall could promote the transport of SO_2 and improve the absorption flux of SO_2 gas. The GO-IM rich in amino improved interfacial compatibility with PVDF. In particular, when the GO-IM was 3% of the PVDF content, the SO_2 absorption flux of the membrane was 6.51×10~(-4) mol/(m~2·s) at test temperature 20 ℃ and feed gas pressure 0.10 MPa, indicating PVDF/GO-IM porous membrane had an excellent application prospect in the field of flue gas desulfurization.
Fossil fuel combustion and automobile exhaust are important sources of PM2.5, and SO_2 is an important component of PM2.5. Membrane contactors show excellent promising in the field of SO_2 removal. In this study, aminated graphene oxide(GO-IM) was synthetized by precipitation polymerization, and then was incorporated into polyvinylidene fluoride(PVDF) to fabricate aminated graphene oxide loaded membrane by immersion precipitation phase transformation. The morphology, porosity, contact angle and mechanical strength of membranes were characterized and the desulfurization performance of membranes was evaluated. In addition, the permeability of PVDF/GO-IM porous membranes with different GO-IM loadings was investigated. The results showed that the aminated graphene oxide on the porous membrane wall could promote the transport of SO_2 and improve the absorption flux of SO_2 gas. The GO-IM rich in amino improved interfacial compatibility with PVDF. In particular, when the GO-IM was 3% of the PVDF content, the SO_2 absorption flux of the membrane was 6.51×10~(-4) mol/(m~2·s) at test temperature 20 ℃ and feed gas pressure 0.10 MPa, indicating PVDF/GO-IM porous membrane had an excellent application prospect in the field of flue gas desulfurization.
引文
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[23] 李颖娜,张玉忠,陈颖,等.气 - 液膜接触器用膜材料的研究进展[J].高分子材料科学与工程,2014,30(8):178-184.
[24] 赵津礼,王建友,张玉忠.新型聚醚砜/磺化聚醚砜共混超滤膜制备方法的研究[J].膜科学与技术,2018,38(4):33-42.
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[27] 李颖娜,李涵,叶卉,等.聚偏氟乙烯一氟化二氧化硅有机 - 无机复合膜的制备及脱硫性能[J].高分子材料科学与工程,2017,33(2):123-129.
[2] Gao X Y,Qiu M H,Fu K Y,et al.Feasibility analysis of SO2 absorption using a hydrophilic ceramic membrane contactor[J].Chin J Chem Eng,2018,26(10):2139-2147.
[3] Fang Z Q,Yu X C,Tang W Q,et al.Denitration by oxidation-absorption with polypropylene hollow fiber membrane contactor[J].Appl Energ,2017,206:858-868.
[4] He F J,Wang T,Fang M X.Screening test of amino acid salts for CO2 absorption at flue gas temperature in a membrane contactor[J].Energ Fuel,2017,31(1):770-777.
[5] Mansourizadeh A,Ismail A F.Hollow fiber gas-liquid membrane contactors for acid gas capture:A review[J].J Hazard Mater,2009,171 (1/3):38-53.
[6] Qi Z,Cussler E L.Microporous hollow fibers for gas absorption:II.Mass transfer across the membrane[J].J Membr Sci,1985,23(3):321-332.
[7] Chang Q,Jia Z Q,Qin J.Progress of membrane gas-liquid contacting process[J].Membr Sci Technol,2012,30(6):106-111.
[8] 李颖娜,张玉忠,刘双龙,等.气 - 液膜接触器法烟气脱硫脱硝的研究进展[J].膜科学与技术,2018,38(5):137-144.
[9] 瞿如敏,沙焱,陈浩,等.聚丙烯中空纤维膜组件分离烟气中的CO2[J].化工进展,2013,32(11):2778-2782.
[10] 徐志摩,陈炜,王建黎,等.膜接触器分离混合气中二氧化碳的研究[J].环境科学,2003,24(5):34-38.
[11] Fougerit V,Pozzobon V,Pareau D,et al.Experimental and numerical investigation binary mixture mass transfer in a gas-liquid membranecontactor[J].J Membr Sci,2019,572:1-11.
[12] Cooney D O,Jackson C C.Gas absorption in a hollow fiber device[J].Chem Eng Commun,1989,79(1):153-163.
[13] Luis P,Garea A,Irabien A.Zero solvent emission process for sulfur dioxide recovery using a membrane contactor and ionic liquids[J].J Membr Sci,2009,330:80-89.
[14] Park H H,Deshwal B R,Kim I W,et al.Absorption of SO2 from flue gas using PVDF hollow fiber membranes in a gas-liquid contactor[J].J Membr Sci,2008,319:29-37.
[15] Jeon H,Ahn H,Song I.Absorption of sulfur dioxide by porous hydrophobic membrane contactor[J].Desalination,2008,234:252-260.
[16] Zhang Z E,Yan Y F,Wood D A.Influence of the membrane module geometry on SO2 removal:A numerical study[J].Ind Eng Chem Res,2015,54:11619-11627.
[17] Yu H S,The J,Tan Z C,et al.Modeling SO2 absorption into water accompanied with reversible reaction in a hollow fiber membrane contactor[J].Chem Eng Sci,2016,156:136-146.
[18] 陈颖,郭春刚,刘国昌,等.膜法海水吸收烟气中二氧化碳的试验研究[J].膜科学与技术,2012,32(1):92-96.
[19] 陈迁乔,钟秦.微孔中空纤维膜接触器烟气脱硫性能的研究[J].高校化学工程学报,2010,24(1):144-149.
[20] 李金伟,黄莉兰,辛清萍,等.醇胺改性氧化石墨烯/PVDF共混膜接触器脱硫性能的研究[J].膜科学与技术,2017,37(6):70-76.
[21] 马玉慧,叶慧,张玉忠,等.聚醚砜中空纤维膜接触器脱硫性能研究[J].膜科学与技术,2016,36(5):60-67.
[22] 李涵,叶卉,王艳兵,等.脱硫用PVDF膜的结构调控与性能研究[J].膜科学与技术,2016,35(1):35-40.
[23] 李颖娜,张玉忠,陈颖,等.气 - 液膜接触器用膜材料的研究进展[J].高分子材料科学与工程,2014,30(8):178-184.
[24] 赵津礼,王建友,张玉忠.新型聚醚砜/磺化聚醚砜共混超滤膜制备方法的研究[J].膜科学与技术,2018,38(4):33-42.
[25] Jr W S H,Offeman R E.Preparation of graphitic oxide[J].J Am Chem soc,1958,80(6):1339.
[26] Xin Q P,Liu H R,Zhang Y,et al.Widening CO2-facilitated transport passageways in SPEEK matrix using polymer brushes functionalized double-shelled organic submicrocapsules for efficient gas separation[J].J Membr Sci,2017,525:330-341.
[27] 李颖娜,李涵,叶卉,等.聚偏氟乙烯一氟化二氧化硅有机 - 无机复合膜的制备及脱硫性能[J].高分子材料科学与工程,2017,33(2):123-129.
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