抗菌聚酰胺复合纳滤膜的制备及表征
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摘要
为了提高复合膜的抗菌性能,以聚砜超滤膜为基膜,以超支化聚乙烯亚胺(PEI)为水相单体,以均苯三甲酰氯(TMC)为有机相单体,制备出PEI/TMC抗菌性聚酰胺复合纳滤膜,并探究复合膜渗透性能和抗菌性能。结果显示:当PEI质量分数为2%、TMC质量分数0.1%、反应时间为5 min时,在1.5 MPa、25℃的条件下过滤0.1%的MgSO_4溶液,得到的膜渗透选择性能最佳,此时通量为55 L/(m~2·h),截留率为95%;以革兰氏阴性菌大肠杆菌以及革兰氏阳性菌金黄色葡萄球菌为细菌模型,采用接触振荡法进行测试,证明了PEI/TMC相比于传统的商品聚酰胺复合膜,具有非常好的抗菌性,对于浓度为10~3CFU/mL左右的细菌,抑菌率可达到70%～95%。
In order to improve the antibacterial property of the composite membrane, an antibacterial composite polyamide nanofiltration membrane was prepared via the interfacial polymerization using the branched polyethyleneimine(PEI) as an aqueous monomer, trimesoyl chloride(TMC) as an organic phase monomer, on the surface of polysulfone ultrafiltration membrane. The effects of different preparation conditions on the membrane properties were studied. It was found that when PEI content was 1.5%, TMC content was 0.2%, reaction time was 5 min, the PEI/TMC composite membrane obtained the best performance. It showed the membrane rejection to 0.1% MgSO_4 was 95%, the flux was about 55 L/(m~2·h) when it was tested at 25 ℃, 1.5 MPa. Gram-negative E. coli and Gram-positive S. aureus were used as the bacterial model to evaluate the antibacterial properties of the membranes using shake flask method. The PEI/TMC membrane has very good antibacterial property and the antibacterial rate reaches 70%-95% for bacteria with a concentration of 10~3 CFU/mL.
In order to improve the antibacterial property of the composite membrane, an antibacterial composite polyamide nanofiltration membrane was prepared via the interfacial polymerization using the branched polyethyleneimine(PEI) as an aqueous monomer, trimesoyl chloride(TMC) as an organic phase monomer, on the surface of polysulfone ultrafiltration membrane. The effects of different preparation conditions on the membrane properties were studied. It was found that when PEI content was 1.5%, TMC content was 0.2%, reaction time was 5 min, the PEI/TMC composite membrane obtained the best performance. It showed the membrane rejection to 0.1% MgSO_4 was 95%, the flux was about 55 L/(m~2·h) when it was tested at 25 ℃, 1.5 MPa. Gram-negative E. coli and Gram-positive S. aureus were used as the bacterial model to evaluate the antibacterial properties of the membranes using shake flask method. The PEI/TMC membrane has very good antibacterial property and the antibacterial rate reaches 70%-95% for bacteria with a concentration of 10~3 CFU/mL.
引文
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[23]LEE K P,ZHENG J,BARGEMAN G,et al.pH stable thin film composite polyamine nanofiltration membranes by interfacial polymerisation[J].Journal of Membrane Science,2015,478:75-84.
[2]GUO W,NGO H H,LI J.A mini-review on membrane fouling[J].Bioresource Technology,2012,122:27-34.
[3]刘兴,邓慧宇.抗污染高分子纳滤膜研究进展[J].膜科学与技术,2018,38(5):113-121.LIU X,DENG H Y.Development of anti-fouling polymeric nanofiltration membrane[J].Membrane Science and Technology,2018,38(5):113-121(in Chinese).
[4]MANSOURI J,HARRISSON S,CHEN V.Strategies for controlling biofouling in membrane filtration systems:Challenges and opportunities[J].Journal of Materials Chemistry,2010(20):4567-4586.
[5]CHENG G,LI G Z,XUE H,et al.Zwitterionic carboxy-betaine polymer surfaces and their resistance to long-term biofilm formation[J].Biomaterials,2009,30:5234-5240.
[6]CHENG G,ZHANG Z,CHEN S,et al.Inhibition of bacterial adhesion and biofilm formation on zwitterionic surfaces[J].Biomaterials,2007,28(29):4192-4199.
[7]LI G Z,CHENG G,XUE H,et al.Ultra low fouling zwitterionic polymers with a biomimetic adhesive group[J].Biomaterials,2008,29:4592-4597.
[8]AYMONIER C,SCHLOTTERBECK U,ANTONIETTI L,et al.Hybrids of silver nanoparticles with amphiphilic hyperbranched macromolecules exhibiting antimicrobial properties[J].Chemical Communications,2002,8(24):3018-3019.
[9]秦龙鑫,潘国元.纳米银在水处理膜中的应用进展[J].化工进展,2016,35(7):2114-2120.QIN L X,PAN G Y.Progress of application of silver nanoparticles in water treatment membranes[J].Chemical Industry and Engineering Progress,2016,35(7):2114-2120(in Chinese).
[10]WALTERS P A,ABBOTT E A,ISQUITH A J.Algicidal activity of a surface-bonded organosilicon quaternary ammonium chloride[J].Applied Microbiology,1973,25(2):253-256.
[11]ANDRESEN M,STENSTAD P,MORETRO T,et al.Non-leaching antimicrobial films prepared from surface modified microfibrillated cellulose[J].Biomacromolecules,2007,8:2149-2155.
[12]JAMES N R,JAYAKRISHNAN J A.Surface thiocyanation of plasticized poly(vinyl chloride)and its effect on bacterial adhesion[J].Biomaterials,2003,24:2205-2212.
[13]张环,陈克宁.应用纳米TiO2整理剂制备抗菌织物及其抗菌性能研究[J].天津工业大学学报,2005,24(6):40-42.ZHANG H,CHEN K N.Preparation of antibacterial fabric by using nano-TiO2as finishing agent and study of its antibacterial properties[J].Journal of Tianjin Polytechnic University,2005,24(6):40-42(in Chinese).
[14]SETIAWAN L,SHI L,WANG R.Dual layer composite nanofiltration hollow fiber membranes for low-pressure water softening[J].Journal of Membrane Science,2013,430(6):129-139.
[15]FREGER V.Nanoscale heterogeneity of polyamide membranes formed by interfacial polymerization[J].Langmuir,2003(19):4791-4797.
[16]杨盛,张宇峰,张艳萍,等.聚哌嗪均苯三甲酰胺纳滤复合膜的研究[J].天津工业大学学报,2008,27(5):8-10.YANG S,ZHANG Y F,ZHANG Y P,et al.Research of polypiperazine amide composite nanofiltration membrane[J].Journal of Tianjin Polytechnic University,2008,27(5):8-10(in Chinese).
[17]LI L,ZHANG S,ZHANG X.Preparation and characterization of poly(piperazineamide)composite nanofiltration membrane by interfacial polymerization of 3,30,5,50-biphenyl tetraacyl chloride and piperazine[J].Journal of Membrane Science,2009,335:133-139.
[18]VERSSIMO S,PEINEMANNK V,BORDADO J.New composite hollow fiber membrane for nanofiltration[J].Desalination,2005(184):1-11.
[19]YANG F,ZHANG S,YANG D,et al.Preparation and characterization of polypiperazine amide/PPESK hollow fiber composite nanofiltration membrane[J].Journal of Membrane Science,2007,301(1/2):85-92.
[20]CHAIG Y,KRANTZ W B.Formation and characterization of polyamide membranes via interfacial polymerization[J].Journal of Membrane Science,1994,93:175-192.
[21]SONG Y,SUN P,HENRY L L.Mechanisms of structure and performance controlled thin film composite membrane formation via interfacial polymerization process[J].Journal of Membrane Science,2005,251(1/2):67-79.
[22]SUBRAMANI A,HOEK E M V.Direct observation of initial microbial deposition onto reverse osmosis and nanofiltration membranes[J].Journal of Membrane Science,2008,319(1/2):111-125.
[23]LEE K P,ZHENG J,BARGEMAN G,et al.pH stable thin film composite polyamine nanofiltration membranes by interfacial polymerisation[J].Journal of Membrane Science,2015,478:75-84.