界面聚合法合成聚酰亚胺渗透汽化膜及表征
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摘要
针对渗透汽化分离二甲基甲酰胺(DMF)和二甲基乙酰胺(DMAc)酰胺类溶剂过程中渗透性和选择性之间此升彼降的矛盾关系(trade-off效应),提出界面聚合薄层PI复合膜的方法。通过均苯四甲酸酐和五氯化磷制备有机相单体均苯四甲酰氯,分别以间苯二胺(MPDA)、丙二胺(DAPE)及己二胺(HMD)为水相单体,采用界面聚合法制备3种耐溶剂型聚酰亚胺(PI)复合膜,并对3种PI复合膜进行表征和渗透汽化分离性能测试。结果表明:3种PI复合膜都具有良好的亲水性、热稳定性;在6种常见的有机溶剂中,保持良好的稳定性;在30～60℃条件下,HMD-PI膜对质量分数90%DMF/H_2O体系和质量分数90%DMAc/H_2O体系的分离因子最高可达12.7和36.8,渗透通量可达1 014和542 g·m~(-2)·h~(-1),具有较好的分离效果。
During pervaporation separation of dimethylformamide(DMF)/water and dimethylacetamide(DMAc)/water systems, a trade-off effect between permeability and selectivity always happens. A method for the synthesis of thin PI composite membranes by interfacial polymerization was proposed for solving this problem. Organic phase monomer pyromellitic chloride(BTAC) was prepared by pyromellitic anhydride and phosphorus pentachloride. Solvent-resistant polyimide(PI) composite membranes were made by interfacial polymerization, where m-phenylenediamine(MPDA), propylenediamine(DAPE) and hexamethylenediamine(HMD) were used as aqueous phase monomers. The PI composite membranes and their pervaporation performance were characterized. All of the three composite membranes had good hydrophilicity and excellent thermal stability. The PI composite membranes presented excellent stabilities after immersing in common organic solvents. When using the HMD-PI membrane to separate solvent/water(90/10 %) from 30 ℃ to 60 ℃,the best separation factor can reach 12.7 and 35.8 for DMF/water and DMAc/water systems respectively, and the flux reaches 1 014 and 542 g·m~(-2)·h~(-1) for DMF/water and DMAc/water systems, respectively. These results indicate that the HMD-PI membrane presents excellent separation performance for solvent/water systems.
During pervaporation separation of dimethylformamide(DMF)/water and dimethylacetamide(DMAc)/water systems, a trade-off effect between permeability and selectivity always happens. A method for the synthesis of thin PI composite membranes by interfacial polymerization was proposed for solving this problem. Organic phase monomer pyromellitic chloride(BTAC) was prepared by pyromellitic anhydride and phosphorus pentachloride. Solvent-resistant polyimide(PI) composite membranes were made by interfacial polymerization, where m-phenylenediamine(MPDA), propylenediamine(DAPE) and hexamethylenediamine(HMD) were used as aqueous phase monomers. The PI composite membranes and their pervaporation performance were characterized. All of the three composite membranes had good hydrophilicity and excellent thermal stability. The PI composite membranes presented excellent stabilities after immersing in common organic solvents. When using the HMD-PI membrane to separate solvent/water(90/10 %) from 30 ℃ to 60 ℃,the best separation factor can reach 12.7 and 35.8 for DMF/water and DMAc/water systems respectively, and the flux reaches 1 014 and 542 g·m~(-2)·h~(-1) for DMF/water and DMAc/water systems, respectively. These results indicate that the HMD-PI membrane presents excellent separation performance for solvent/water systems.
引文
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[2]JIANG L Y,WANG Y,CHUNG T S,et al.Polyimides membranes for pervaporation and biofuels separation[J].Progress in Polymer Science,2009,34(11):1135-1160.
[3]HERMANS S,MARIEN H,et al.Recent developments in thin film(nano)composite membranes for solvent resistant nanofiltration[J].Current Opinion in Chemical Engineering,2015,8:45-54.
[4]XU R,GUO M,WANG J,et al.Fabrication of solvent-resistant copolyimide membranes for pervaporation recovery of amide solvents[J].Chemical Engineering&Technology,2018,41(2):337-344.
[5]邓力,马文中,徐荣,等.均苯型耐酰胺溶剂聚酰亚胺膜渗透汽化性能研究[J].高校化学工程学报,2018,32(3):537-544.DENG L,MA W Z,XU R,et al.Study on pervaporation performance of amide resistance polypyromellitimde membranes[J].Journal of Chemical Engineering of Chinese Universities,2018,32(3):537-544.
[6]XU S,LIU L F,WANG Y.Network cross-linking of polyimide membranes for pervaporation dehydration[J].Separation&Purification Technology,2017,185:215-226.
[7]RAAIJMAKERS M J T,BENES N E.Current trends in interfacial polymerization chemistry[J].Progress in Polymer Science,2016,63:86-142.
[8]杨振生,张磊,张广厚,等.界面聚合法PI/PP耐溶剂复合纳滤膜的制备与表征[J].化工学报,2012,63(8):2635-2641.YANG Z S,ZHANG L,ZHANG G H,et al.Preparation and characterization of polyimide/po-lypropylene solvent resistant nanofiltration composite membrane via interfacial polymerization[J].Journal of Chemical Industry and Engineering,2012,63(8):2635-2641.
[9]HUANG S H,LIU Y Y,HUANG Y H,et al.Study on characterization and pervaporation performance of interfacially polymerized polyamide thin-film composite membranes for dehydrating tetrahydrofuran[J].CIESC Journal,2014,470(23):411-420.
[10]YANG S S,ZHEN H Y,SU B W.Polyimide thin film composite(TFC)membranes via interfacial polymerization on hydrolyzed polyacrylonitrile support for solvent resistant nanofiltration[J].Rsc Advances,2017,7(68):42800-42810.
[11]CHERN Y T,CHEN L W.Interfacial polyfunctional condensation:effect of the reaction conditions[J].Journal of Applied Polymer Science,2010,42(9):2543-255.
[12]BRANDRUP J,IMMERGUT E H,GRULKE E A.Polymer handbook[M].New York:John Wily&Sons,Inc.1999.
[13]TANG J,SIRKAR K K.Perfluoropolymer membrane behaves like a zeolite membrane in dehydration of aprotic solvents[J].Journal of Membrane Science,2012,421:211-216.
[14]TANG J,SIRKAR K K,MAJUMDAR S.Pervaporative dehydration of concentrated aqueous solutions of selected polar organics by a perfluoropolymer membrane[J].Separation and Purification Technology,2017,175:122-129.
[15]KIM J H,LEE K H,KIM S Y.Pervaporation separation of water from ethanol through polyimide composite membranes[J].Journal of Membrane Science,2000,169(1):81-93.
[16]SOLAK E K,ASMAN G,?AMURLU P,et al.Sorption,diffusion,and pervaporation characteristics of dimethylformamide/water mixtures using sodium alginate/polyvinyl pyrrolidone blend membranes[J].Vacuum,2008,82(6):579-587.
[17]DAS S,BANTHIA A K,ADHIKARI B.Pervaporation separation of DMF from water using a crosslinked polyurethane urea-PMMAIPN membrane[J].Desalination,2006,197(1/2/3):106-116.