表面改性纳米氧化铝亲水共混膜制备及其水处理效能
|
摘要
经低温等离子体处理后,在纳米氧化铝(Al_2O_3)表面接枝甲基丙烯酸-2-羟乙酯(HEMA)或其聚合物,制备了Al_2O_3-g-HEMA纳米复合颗粒。采用纳米Al_2O_3及Al_2O_3-g-HEMA纳米复合颗粒分别与聚偏氟乙烯(PVDF)共混,制备了PVDF/Al_2O_3膜和PVDF/Al_2O_3-g-HEMA膜,并与未改性PVDF膜进行比较。考察了改性纳米Al_2O_3表面的接枝情况和平均粒径,以及上述3种超滤膜处理聚驱采油废水的通量、出水水质及膜污染情况。结果表明,经表面改性的纳米Al_2O_3,其颗粒团聚得到良好控制,平均粒径大幅下降。PVDF/Al_2O_3膜和PVDF/Al_2O_3-g-HEMA膜的亲水性、纯水通量、处理聚驱采油废水的运行通量及清洗后通量恢复率均大幅提高。3种膜对聚丙烯酰胺、油类和TOC均有良好的去除效果,且共混改性不影响膜对大分子物质的去除。以PVDF/Al_2O_3-g-HEMA纳米复合颗粒作为添加剂制备的共混膜,其通量、去除效果和抗污染能力等综合性能最佳,是深度处理聚驱采油废水的理想膜材料。
Al_2O_3-g-HEMA nanocomposites were prepared by grafting HEMA or its polymers onto the surface of alumina nanoparticles through low temperature plasma. Two kinds of modified PVDF ultrafiltration membranes were prepared by blending alumina nanoparticles or surface modified alumina nanoparticles in the membrane matrix. The raw PVDF ultrafiltration membrane without nanoparticles were set as the control group. The graft efficiency and the extent of reduction on nanoparticle agglomeration was evaluated. The change of flux,permeate quality and membrane fouling of the prepared membranes were also investigated when applied in polymer flooding wastewater treatment. Results showed that a good graft effect had been achieved. The surface modified alumina nanoparticles had a significant drop on the average particle diameter,which meant an evident decrease on the nanoparticle agglomeration. The hydrophilicity and pure water flux of PVDF/Al_2O_3 mixed matrix membranes and PVDF/Al_2O_3-g-HEMA mixed matrix membranes were significantly higher. Meanwhile,the operation flux and the recovery ratio after physical cleaning were enhanced in treating polymer flooding wastewater. All the modified membranes prepared shared similarly good performance in the treatment of polymer flooding wastewater compared to the control group. Analysis and comparison on the molecular weight of contaminants in the influent and effluent proved an unaltered removal efficiency of macromolecule for the modified membranes. PVDF membranes blended with Al_2O_3-g-HEMA nanocomposites shows best comprehensive performance in flux,rejection ability and anti-fouling property. It is a superior membrane material in advanced treatment of polymer flooding wastewater.
Al_2O_3-g-HEMA nanocomposites were prepared by grafting HEMA or its polymers onto the surface of alumina nanoparticles through low temperature plasma. Two kinds of modified PVDF ultrafiltration membranes were prepared by blending alumina nanoparticles or surface modified alumina nanoparticles in the membrane matrix. The raw PVDF ultrafiltration membrane without nanoparticles were set as the control group. The graft efficiency and the extent of reduction on nanoparticle agglomeration was evaluated. The change of flux,permeate quality and membrane fouling of the prepared membranes were also investigated when applied in polymer flooding wastewater treatment. Results showed that a good graft effect had been achieved. The surface modified alumina nanoparticles had a significant drop on the average particle diameter,which meant an evident decrease on the nanoparticle agglomeration. The hydrophilicity and pure water flux of PVDF/Al_2O_3 mixed matrix membranes and PVDF/Al_2O_3-g-HEMA mixed matrix membranes were significantly higher. Meanwhile,the operation flux and the recovery ratio after physical cleaning were enhanced in treating polymer flooding wastewater. All the modified membranes prepared shared similarly good performance in the treatment of polymer flooding wastewater compared to the control group. Analysis and comparison on the molecular weight of contaminants in the influent and effluent proved an unaltered removal efficiency of macromolecule for the modified membranes. PVDF membranes blended with Al_2O_3-g-HEMA nanocomposites shows best comprehensive performance in flux,rejection ability and anti-fouling property. It is a superior membrane material in advanced treatment of polymer flooding wastewater.
引文
[1]郭海成,肖蓝,于水利.原油乳化液对阴离子交换膜的污染特征[J].中国给水排水,2014,30(13):37-41.Guo Haicheng,Xiao Lan,Yu Shuili.Characterization of anion exchange membrane fouling by oil emulsion[J].China Water&Wastewater,2014,30(13):37-41(in Chinese).
[2]徐俊,贾凌志,孙勇,等.改性聚偏氟乙烯超滤膜深度处理采油污水[J].中国给水排水,2010,26(1):74-76.Xu Jun,Jia Lingzhi,Sun Yong,et al.Advanced treatment of oilfield produced wastewater by modified polyvinylidene fluoride ultrafiltration membrane[J].China Water&Wastewater,2010,26(1):74-76(in Chinese).
[3]孙欣,王鹏,赵姗姗.混凝-超滤处理聚驱采油废水工艺研究[J].哈尔滨商业大学学报:自然科学版,2013,29(2):176-179.Sun Xin,Wang Peng,Zhao Shanshan.Study on coagulation-ultrafiltration technology for treatment of oilfield polymer flooding produced water[J].Journal of Harbin University of Commerce:Natural Science Edition,2013,29(2):176-179(in Chinese).
[4]Ahmadun F R,Pendashteh A,Abdullah L C,et al.Review of technologies for oil and gas produced water treatment[J].J Hazard Mater,2009,170(2):530-551.
[5]Guo H,Xiao L,Yu S,et al.Analysis of anion exchange membrane fouling mechanism caused by anion polyacrylamide in electrodialysis[J].Desalination,2014,346:46-53.
[6]Zhang R,Shi W,Yu S,et al.Influence of salts,anion polyacrylamide and crude oil on nanofiltration membrane fouling during desalination process of polymer flooding produced water[J].Desalination,2015,373:27-37.
[7]李文国,王乐译,张伟政,等.PVDF膜污染控制及清洗方法探讨[J].水处理技术,2014,40(3):91-93.Li Wenguo,Wang Leyi,Zhang Weizheng,et al.PVDFmembrane fouling control and cleaning method discussion[J].Water Treatment Technology,2014,40(3):91-93(in Chinese).
[8]王彪,王志明,徐卫华,等.管式超滤膜处理油田采出水过程中膜污染分析及对策[J].水处理技术,2010,36(6):50-53.Wang Biao,Wang Zhiming,Xu Weihua,et al.Analysis and countermeasures of membrane fouling in the process of dealing with the oilfield produced water by using pipe ultrafiltration membrane[J].Water Treatment Technology,2010,36(6):50-53(in Chinese).
[9]Lu Y,Yu S L,Chai B X,et al.Effect of nano-sized Al2O3-particle addition on PVDF ultrafiltration membrane performance[J].J Membr Sci,2006,276(1):162-167.
[10]Zhang G,Lu S,Zhang L,et al.Novel polysulfone hybrid ultrafiltration membrane prepared with Ti O2-g-HEMAand its antifouling characteristics[J].J Membr Sci,2013,436:163-173.
[11]Abboud M,Turner M,Duguet E,et al.PMMA-based composite materials with reactive ceramic fillers.Part 1:Chemical modification and characterisation of ceramic particles[J].J Mater Chem,1997,7(8):1527-1532.
[12]Arthanareeswaran G,Thanikaivelan P.Fabrication of cellulose acetate-zirconia hybrid membranes for ultrafiltration applications:Performance,structure and fouling analysis[J].Sep Purif Technol,2010,74(2):230-235.
[13]Park H B,Kamcev J,Robeson L M,et al.Maximizing the right stuff:The trade-off between membrane permeability and selectivity[J].Science,2017,356(6343):1138-1148.
[14]Zhang B,Yu S,Zhu Y,et al.Application of a polytetrafluoroethylene(PTFE)flat membrane for the treatment of pre-treated ASP flooding produced water in a Daqing oilfield[J].RSC Adv,2016,67(6):62411-62419.
[15]Vasanth D,Pugazhenthi G,Uppaluri R.Cross-flow microfiltration of oil-in-water emulsions using low cost ceramic membranes[J].Desalination,2013,320(11):86-95.
[16]Huang W,Chu H,Dong B.Characteristics of algogenic organic matter generated under different nutrient conditions and subsequent impact on microfiltration membrane fouling[J].Desalination,2012,293:104-111.
[2]徐俊,贾凌志,孙勇,等.改性聚偏氟乙烯超滤膜深度处理采油污水[J].中国给水排水,2010,26(1):74-76.Xu Jun,Jia Lingzhi,Sun Yong,et al.Advanced treatment of oilfield produced wastewater by modified polyvinylidene fluoride ultrafiltration membrane[J].China Water&Wastewater,2010,26(1):74-76(in Chinese).
[3]孙欣,王鹏,赵姗姗.混凝-超滤处理聚驱采油废水工艺研究[J].哈尔滨商业大学学报:自然科学版,2013,29(2):176-179.Sun Xin,Wang Peng,Zhao Shanshan.Study on coagulation-ultrafiltration technology for treatment of oilfield polymer flooding produced water[J].Journal of Harbin University of Commerce:Natural Science Edition,2013,29(2):176-179(in Chinese).
[4]Ahmadun F R,Pendashteh A,Abdullah L C,et al.Review of technologies for oil and gas produced water treatment[J].J Hazard Mater,2009,170(2):530-551.
[5]Guo H,Xiao L,Yu S,et al.Analysis of anion exchange membrane fouling mechanism caused by anion polyacrylamide in electrodialysis[J].Desalination,2014,346:46-53.
[6]Zhang R,Shi W,Yu S,et al.Influence of salts,anion polyacrylamide and crude oil on nanofiltration membrane fouling during desalination process of polymer flooding produced water[J].Desalination,2015,373:27-37.
[7]李文国,王乐译,张伟政,等.PVDF膜污染控制及清洗方法探讨[J].水处理技术,2014,40(3):91-93.Li Wenguo,Wang Leyi,Zhang Weizheng,et al.PVDFmembrane fouling control and cleaning method discussion[J].Water Treatment Technology,2014,40(3):91-93(in Chinese).
[8]王彪,王志明,徐卫华,等.管式超滤膜处理油田采出水过程中膜污染分析及对策[J].水处理技术,2010,36(6):50-53.Wang Biao,Wang Zhiming,Xu Weihua,et al.Analysis and countermeasures of membrane fouling in the process of dealing with the oilfield produced water by using pipe ultrafiltration membrane[J].Water Treatment Technology,2010,36(6):50-53(in Chinese).
[9]Lu Y,Yu S L,Chai B X,et al.Effect of nano-sized Al2O3-particle addition on PVDF ultrafiltration membrane performance[J].J Membr Sci,2006,276(1):162-167.
[10]Zhang G,Lu S,Zhang L,et al.Novel polysulfone hybrid ultrafiltration membrane prepared with Ti O2-g-HEMAand its antifouling characteristics[J].J Membr Sci,2013,436:163-173.
[11]Abboud M,Turner M,Duguet E,et al.PMMA-based composite materials with reactive ceramic fillers.Part 1:Chemical modification and characterisation of ceramic particles[J].J Mater Chem,1997,7(8):1527-1532.
[12]Arthanareeswaran G,Thanikaivelan P.Fabrication of cellulose acetate-zirconia hybrid membranes for ultrafiltration applications:Performance,structure and fouling analysis[J].Sep Purif Technol,2010,74(2):230-235.
[13]Park H B,Kamcev J,Robeson L M,et al.Maximizing the right stuff:The trade-off between membrane permeability and selectivity[J].Science,2017,356(6343):1138-1148.
[14]Zhang B,Yu S,Zhu Y,et al.Application of a polytetrafluoroethylene(PTFE)flat membrane for the treatment of pre-treated ASP flooding produced water in a Daqing oilfield[J].RSC Adv,2016,67(6):62411-62419.
[15]Vasanth D,Pugazhenthi G,Uppaluri R.Cross-flow microfiltration of oil-in-water emulsions using low cost ceramic membranes[J].Desalination,2013,320(11):86-95.
[16]Huang W,Chu H,Dong B.Characteristics of algogenic organic matter generated under different nutrient conditions and subsequent impact on microfiltration membrane fouling[J].Desalination,2012,293:104-111.