新型PEI/PAA复合正渗透膜的制备及性能表征
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摘要
采用聚乙烯亚胺(PEI)和聚丙烯酸(PAA)分别作为聚阴阳电解质,间苯二胺(MPD)与均苯三甲酰氯(TMC)分别为水相和油相单体,依次采用层层自组装(LBL)和界面聚合的方法对聚丙烯腈(PAN)基膜进行改性,探究层层自组装和界面聚合条件对膜性能的影响,并制备新型复合正渗透膜.得出最佳制备条件为:PAA与PEI的沉积时间为10 min,浓度为1 g·L~(-1),pH分别为9和3,支撑盐浓度为1.5 mol·L~(-1),MPD浓度为20 g·L~(-1),水相沉积时间为2 min,TMC浓度为1 g·L~(-1),界面聚合反应时间为60 s,聚电解质层数为2层,在此条件下制得的复合正渗透膜性能优良.以去离子水作为原液,1 mol·L~(-1) NaCl作为汲取液,水通量最高可达26.12 L·m~(-2)·h~(-1),反向盐通量为13.08 g·m~(-2)·h~(-1),与基膜相比,复合膜的亲水性能明显提高,抗污染性能提高,为正渗透膜的制备提供了新的方法和思路.
A novel forward osmosis membrane was fabricated through layer-by-layer(LBL) assembly technology and then interfacial polymerization(IP) method with polyacrylonitrile(PAN) as substrate material in this study. The influences of LBL and IP conditions on the properties of membranes were investigated in detail. Polyethyleneimine(PEI) and polyacrylic acid(PAA) were used as the cationic and anionic polyelectrolytes. M-phenylenediamine(MPD) and 1,3,5-benzenetricarbonyl trichloride(TMC) were used as monomers in water and oil phase, respectively. The optimum preparation conditions were obtained as follows. The deposition time and concentration of PAA and PEI were all 10 min and 1 g·L~(-1). The pH for PAA and PEI were 9 and 3, respectively. The concentration of sodium chloride was 1.5 mol·L~(-1). 20 g·L~(-1) MPD aqueous solution was firstly deposited on membrane for 2 min and then followed by interfacial polymerization of 1 g·L~(-1) TMC for 60 s. The optimum polyelectrolyte layer was 2 layers. In this condition, the water flux of 26.12 L·m~(-2)·h~(-1) and the reverse salt flux of 13.08 g·m~(-2)·h~(-1) were achieved by the composite forward osmosis membrane with deionized water as the raw solution and 1 mol·L~(-1) NaCl as the draw solution. Compared with the base film, the hydrophilic property and anti-fouling property of composite membrane were obviously improved, which provided a new approach for the preparation of forward osmosis membrane.
A novel forward osmosis membrane was fabricated through layer-by-layer(LBL) assembly technology and then interfacial polymerization(IP) method with polyacrylonitrile(PAN) as substrate material in this study. The influences of LBL and IP conditions on the properties of membranes were investigated in detail. Polyethyleneimine(PEI) and polyacrylic acid(PAA) were used as the cationic and anionic polyelectrolytes. M-phenylenediamine(MPD) and 1,3,5-benzenetricarbonyl trichloride(TMC) were used as monomers in water and oil phase, respectively. The optimum preparation conditions were obtained as follows. The deposition time and concentration of PAA and PEI were all 10 min and 1 g·L~(-1). The pH for PAA and PEI were 9 and 3, respectively. The concentration of sodium chloride was 1.5 mol·L~(-1). 20 g·L~(-1) MPD aqueous solution was firstly deposited on membrane for 2 min and then followed by interfacial polymerization of 1 g·L~(-1) TMC for 60 s. The optimum polyelectrolyte layer was 2 layers. In this condition, the water flux of 26.12 L·m~(-2)·h~(-1) and the reverse salt flux of 13.08 g·m~(-2)·h~(-1) were achieved by the composite forward osmosis membrane with deionized water as the raw solution and 1 mol·L~(-1) NaCl as the draw solution. Compared with the base film, the hydrophilic property and anti-fouling property of composite membrane were obviously improved, which provided a new approach for the preparation of forward osmosis membrane.
引文
And M A,Goh M C.1999.In situ investigations of polyelectrolyte film formation by second harmonic generation[J].Journal of Physical Chemistry B,103(49):10729-10732
方鹏,曹兵,淡宜,等.2011.界面聚合法制备聚酰胺纳滤膜及工艺条件对纳滤膜性能的影响[J].高分子材料科学与工程,27(10):1-3
高克,许中煌,洪昱斌,等.2017.氧化石墨烯-陶瓷复合纳滤膜的层层自组装制备及其性能[J].化工学报,68(5):2177-2185
Gao M,Zhang X,Yang B,et al.1996.Assembly of modified CdS particles/cationic polymer based on electrostatic interactions[J].Thin Solid Films,s284-285(2):242-245
Qiu C,Qi S,Tang C Y.2011.Synthesis of high flux forward osmosis membranes by chemically crosslinked layer-by-layer polyelectrolytes[J].Journal of Membrane Science,381(1):74-80
Rahimpour A,Jahanshahi M,Mortazavian N,et al.2010.Preparation and characterization of asymmetric polyethersulfone and thin-film composite polyamide nanofiltration membranes for water softening[J].Applied Surface Science,256(6):1657-1663
唐媛媛,徐佳,陈幸,等.2015.正渗透脱盐过程的核心—正渗透膜[J].化学进展,27(7):818-830
陶杰,何平,夏敏玲,等.2010.芳香聚酰胺反渗透复合膜的抗氧化性能研究[J].水处理技术,36(3):42-45
王波,文湘华,申博,等.2016.正渗透技术研究现状及进展[J].环境科学学报,36(9):3118-3126
王磊,呼佳瑞,苗瑞,等.2014.聚酰胺复合纳滤膜的制备与表征[J].膜科学与技术,34(5):16-21
Wang R,Shi L,Tang C Y,et al.2010.Characterization of novel forward osmosis hollow fiber membranes[J].Journal of Membrane Science,355(1):158-167
韦希,周雪飞,褚华强.2016.正渗透膜在水处理应用中的研究进展[J].水处理技术,42(3):13-19
杨盛,张宇峰,张艳萍,等.2008.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,27(5):8-10
俞昌朝,储月霞,沈江南,等.2014.纳米碳管改性聚哌嗪酰胺复合纳滤膜的制备[J].高校化学工程学报,28(1):84-91
Zhang G,Yan H,Ji S,et al.2007.Self-assembly of polyelectrolyte multilayer pervaporation membranes by a dynamic layer-by-layer technique on a hydrolyzed polyacrylonitrile ultrafiltration membrane[J].Journal of Membrane Science,292(1):1-8
Zhao S,Zou L,Tang C Y,et al.2012.Recent developments in forward osmosis: Opportunities and challenges[J].Journal of Membrane Science,396(1):1-21
方鹏,曹兵,淡宜,等.2011.界面聚合法制备聚酰胺纳滤膜及工艺条件对纳滤膜性能的影响[J].高分子材料科学与工程,27(10):1-3
高克,许中煌,洪昱斌,等.2017.氧化石墨烯-陶瓷复合纳滤膜的层层自组装制备及其性能[J].化工学报,68(5):2177-2185
Gao M,Zhang X,Yang B,et al.1996.Assembly of modified CdS particles/cationic polymer based on electrostatic interactions[J].Thin Solid Films,s284-285(2):242-245
Qiu C,Qi S,Tang C Y.2011.Synthesis of high flux forward osmosis membranes by chemically crosslinked layer-by-layer polyelectrolytes[J].Journal of Membrane Science,381(1):74-80
Rahimpour A,Jahanshahi M,Mortazavian N,et al.2010.Preparation and characterization of asymmetric polyethersulfone and thin-film composite polyamide nanofiltration membranes for water softening[J].Applied Surface Science,256(6):1657-1663
唐媛媛,徐佳,陈幸,等.2015.正渗透脱盐过程的核心—正渗透膜[J].化学进展,27(7):818-830
陶杰,何平,夏敏玲,等.2010.芳香聚酰胺反渗透复合膜的抗氧化性能研究[J].水处理技术,36(3):42-45
王波,文湘华,申博,等.2016.正渗透技术研究现状及进展[J].环境科学学报,36(9):3118-3126
王磊,呼佳瑞,苗瑞,等.2014.聚酰胺复合纳滤膜的制备与表征[J].膜科学与技术,34(5):16-21
Wang R,Shi L,Tang C Y,et al.2010.Characterization of novel forward osmosis hollow fiber membranes[J].Journal of Membrane Science,355(1):158-167
韦希,周雪飞,褚华强.2016.正渗透膜在水处理应用中的研究进展[J].水处理技术,42(3):13-19
杨盛,张宇峰,张艳萍,等.2008.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,27(5):8-10
俞昌朝,储月霞,沈江南,等.2014.纳米碳管改性聚哌嗪酰胺复合纳滤膜的制备[J].高校化学工程学报,28(1):84-91
Zhang G,Yan H,Ji S,et al.2007.Self-assembly of polyelectrolyte multilayer pervaporation membranes by a dynamic layer-by-layer technique on a hydrolyzed polyacrylonitrile ultrafiltration membrane[J].Journal of Membrane Science,292(1):1-8
Zhao S,Zou L,Tang C Y,et al.2012.Recent developments in forward osmosis: Opportunities and challenges[J].Journal of Membrane Science,396(1):1-21