面向油水分离的无机膜制备及应用进展
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摘要
膜技术是处理含油污水及含水油液的有效分离方法。无机膜材料由于可调变的表面性质和良好的稳定性,即使在苛刻的条件下,在分离油水方面表现出优异的分离性能。本文首先阐述了设计与制备油水分离膜的理论基础,包括分离过程中压力驱动力和膜表面特性对膜通量和选择性的影响;然后综述了当前国内外用于油水分离的无机膜的制备及其应用进展,重点介绍分子筛膜、金属氧化物/金属氢氧化物膜和氧化石墨烯膜等的研究,分析了在不同油水混合物中研究者们调控无机膜表面性能的策略,提出膜表面润湿性和膜结构是提高膜分离效率和抗污染性的关键;最后指出抵制含大量表面活性剂、碱液及有机聚合物种的乳化油对膜造成污染,是无机膜亟需解决的问题,并展望了无机膜在分离油水方面的发展方向。
Membrane-based technologies are every effective for the separation of oil/water systems. Because of the controllable surface properties and excellent stability, inorganic membrane particularly has great potential for the oil-water separation even under harsh conditions. First, the theoretical basis of the design and preparation of oil-water separation membrane was described in this paper.Factors that are significantly affects membrane flux and selectivity were analyzed. Then, recent progress of preparation and application of inorganic membranes for the oil-water system, with special highlights on zeolite, metal oxide, graphene oxide membranes,was reviewed. It is concluded that the surface wetting properties and membrane structure are the key to improve separation efficiency and the anti-fouling properties. Controlling membrane fouling is of significant importance for application of inorganic membranes to separation of oil/water emulsions, particularly with the presence of surfactants, alkaline and organic polymers. Finally, future directions on the development of application inorganic membranes for separation of oil/water mixtures were also briefly discussed.
Membrane-based technologies are every effective for the separation of oil/water systems. Because of the controllable surface properties and excellent stability, inorganic membrane particularly has great potential for the oil-water separation even under harsh conditions. First, the theoretical basis of the design and preparation of oil-water separation membrane was described in this paper.Factors that are significantly affects membrane flux and selectivity were analyzed. Then, recent progress of preparation and application of inorganic membranes for the oil-water system, with special highlights on zeolite, metal oxide, graphene oxide membranes,was reviewed. It is concluded that the surface wetting properties and membrane structure are the key to improve separation efficiency and the anti-fouling properties. Controlling membrane fouling is of significant importance for application of inorganic membranes to separation of oil/water emulsions, particularly with the presence of surfactants, alkaline and organic polymers. Finally, future directions on the development of application inorganic membranes for separation of oil/water mixtures were also briefly discussed.
引文
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[19]袁腾,陈卓,周显宏,等.基于超亲水超疏油原理的网膜及其在油水分离中的应用[J].化工学报, 2014, 65(6):1943-1951.YUAN Teng, CHEN Zhuo, ZHOU Xianhong, et al. Coated mesh film basedonsuperhydrophilicandsuperoleophobicprincipleandits applicationinoil-waterseparation[J].CIESCJournal,2014,65(6):1943-1951.
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[22]ERBILHY,DEMIRELAL,AVCIY,etal.Transformationofa simpleplasticintoasuperhydrophobicsurface[J].Science,2003,299(5611):1377-1380.
[23]VOGLEREA.Structureandreactivityofwateratbiomaterial surfaces[J]. Adv. Colloid Interface Sci., 1998, 74:69-117.
[24]ZHANG W, LIU N, CAO Y. et al. Superwetting porous materials for wastewater treatment:from immiscible oil/water mixture to emulsion separation[J]. Adv. Mater. Interfaces, 2017, 4(10):1700029.
[25]MIWAM,NAKAJIMAA,FUJISHIMAA,etal.Effectsofthe surfaceroughnessonslidinganglesofwaterdropletson superhydrophobic surfaces[J]. Langmuir, 2000, 16:5754-5760.
[26]CUIJ,ZHANGX,LIUH,etal.Preparationandapplicationof zeolite/ceramicmicrofiltrationmembranesfortreatmentofoil contaminated water[J]. J. Membr. Sci., 2008, 325(1):420-426.
[27]SCHEIBLERJR,SANTOSERF,BARBOSAAS,etal.Performanceofzeolitemembrane(ZSM-5/γ-Alumina)inthe oil/waterseparationprocess[J].Desalin.WaterTreat.,2015,56(13):3561-3567.
[28]WEN Q, DI J, JIANG L, et al. Zeolite-coated mesh film for efficient oil–water separation[J]. Chem. Sci., 2013, 4:591-595.
[29]ZENG J, GUO Z. Superhydrophilic and underwater superoleophobic MFI zeolite-coated film for oil/water separation[J]. Colloids Surf. A,2014, 444:283-288.
[30]LIUR,DANGWALS,SHAIKI,etal.Hydrophilicity-controlled MFI-typezeolite-coatedmesh for oil/waterseparation[J].Sep.Purif.Technol., 2018, 195:163-169.
[31]于吉红,温强,邸建城,等.一种无机相分离膜及其在油水分离中的应用:CN201210086896.0[P]. 2012-03-29.YUJihong,WENQiang,DIJiancheng,etal.Inorganicphase separation membrane and application thereof in oil-water separation:CN201210086896.0[P]. 2012-03-29.
[32]ZHANGF,ZHANGWB,SHIZ,etal.Nanowire-hairedinorganic membraneswithsuperhydrophilicityandunderwaterultralow adhesivesuperoleophobicityforhigh-efficiencyoil/waterseparation[J]. Adv. Mater., 2013, 2:4192-4198.
[33]LIU N, CHEN Y, LU F, et al. Straightforward oxidation of a copper substrate produces an underwater superoleophobic mesh for oil/water separation[J]. Chem. Phys. Chem., 2013, 14(15):3489-3494.
[34]WANG K, HAN D S, YIMING W, et al. A windable and stretchable three-dimensionalall-inorganicmembraneforefficientoil/water Separation[J]. Sci. Rep., 2017, 7:16081.
[35]LIJ,YANL,HUW,etal.Facilefabricationofunderwater superoleophobicTi O2coatedmeshforhighlyefficientoil/water separation[J]. Colloids Surf. A, 2016, 489:441-446.
[36]LIUN,LINX,ZHANGW,etal.ApureinorganicZnO-Co3O4overlapped membrane for efficient oil/water emulsions separation[J].Sci. Rep., 2015, 5:9688.
[37]李方,孟蝶.氧化石墨烯:膜科学的机遇与挑战[J].膜科学与技术, 2015, 35(6):106-112.LIFang,MENGDie,Grapheneoxide:challengesandopportunities for membrane science[J]. Membr. Sci. Techno., 2015, 35(6):106-112.
[38]HUANGY,LIH,WANGL,etal.Ultrafiltrationmembraneswith structure-optimized graphene-oxide coatings for antifouling oil/water separation[J]. Adv. Mater. Interfaces, 2015, 2:1400433.
[39]DONGY,LIJ,SHIL,etal.Underwatersuperoleophobicgraphene oxidecoatedmeshesfortheseparationofoilandwater[J].Chem.Comm., 2014, 50:5586.
[40]AOC,YUANW,ZHAOJ,etal.Superhydrophilicgraphene oxide@electrospuncellulosenanofiberhybridmembranefor high-efficiency oil/water separation[J]. Carbohyd. Polym., 2017, 175:216-222.
[41]GE J, SHI L, WANG Y, et al. Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill[J]. Nature Nanotech.,2017, 12:434-441.
[42]QIUS,HOUL,LIUJ.High-fluxcontinuousoilspillcollectionby usingahydrophobic/oleophilicnanofibrouscontainer[J].RSCAdv.,2017, 7:19434-19438.
[43]LIJ,XUC,ZHANGY,etal.Gravity-directedseparationofboth immiscibleandemulsifiedoil/watermixturesutilizingcoconutshell layer[J]. J. Colloid Interface Sci., 2018, 211:233-242.
[44]LUD,ZHANGT,GUTIERREZL,etal.Influenceofsurface propertiesoffiltration-layermetaloxideonceramicmembrane foulingduringultrafiltrationofoil/wateremulsion[J].Environ.Sci.Technol., 2016, 50:4668-4674.
[45]ZHAOX,CHENW,SUY,etal.Hierarchicallyengineered membranesurfaceswithsuperiorantifoulingandself-cleaning properties[J]. J. Membr. Sci., 2013, 441:93-101.
[2]樊栓狮,王金渠.无机膜处理含油废水[J].大连理工大学学报,2000, 40(1):61-63.FAN Shuanshi, WANG Jinqu.Treatment of oil-containing wastewater with an inorganic membrane[J].J. Dalian Univ. Techno., 2000, 40(1):61-63.
[3]徐南平,邢卫红,王沛,等.无机膜在工业废水处理中的应用与展望[J].膜科学与技术, 2000, 20(3):23-28.XUNanping,XINGWeihong,WANGPei,etal.Thedevelopment and application of inorganic membranes in the treatment of industrial waste water[J]. Membr. Sci. Techno., 2000, 20(3):23-28.
[4]王枢,褚良银,陈文梅,等.油水分离膜的研究新进展[J].油田化学, 2003, 20(4):387-390.WANGShu,CHULiangyin,CHENWenmei,etal.Advancesin researchesonoil/waterseparationmembranes[J].OilfieldChem., 2003, 20(4):387-390.
[5]WANG B, LIANG W, GUO Z, et al. Biomimetic super-lyophobic and super-lyophilicmaterialsappliedforoil/waterseparation:anew strategy beyond nature[J]. Chem. Soc. Rev., 2015, 44(1):336-361.
[6]GUPTA R K, DUNDERDALE G J, ENGLAND M W, et al. Oil/water separationtechniques:areviewofrecentprogressesandfuture directions[J]. J. Mater. Chem. A, 2017, 5:16025-16058.
[7]董哲勤,王宝娟,许振良,等.油水分离功能膜制备技术研究进展[J].化工进展, 2017, 36(1):1-9.DONGZheqin,WANGBaojuan,XUZhenliang,etal.Recent progressonfabricationtechnologyoffunctionalmembranesfor oil/water separation[J]. Chem. Ind. Eng. Prog., 2017, 36(1):1-9.
[8]ZHUQ,CHUY,WANGZ,etal.Robustsuperhydrophobic polyurethane sponge as a highly reusable oil-absorption material[J]. J.Mater. Chem. A, 2013, 1:5386-5393.
[9]CALCAGNILE P, FRAGOULI D, BAYER I S, et al. Driven floating foams for the removal of oil contaminants from water[J]. ACS Nano,2012, 6(6):5413-5419.
[10]YUEZ,ECONOMYJ.nanoparticleandnanoporouscarbon adsorbents for removal of trace organic contaminants from water[J]. J.Nanopart. Res., 2005, 7:477-487.
[11]XUEZ,WANGS,LINL,etal.Anovelsuperhydrophilicand underwatersuperoleophobichydrogel-coatedmeshforoil/water separation[J]. Adv. Mater., 2011, 23:4270-4273.
[12]ZHANGL,ZHANGZ,WANGP.Smartsurfaceswithswitchable superoleophilicityandsuperoleophobicitinaqueousmedia:toward controllable oil/water separation[J]. NPG Asia Materials, 2012, 4:1-7.
[13]TIAN D, ZHANG X, TIAN Y, et al. Photo-induced water-oil separation basedonswitchablesuperhydrophobicity-superhydrophilicityand underwater superoleophobicity of the aligned ZnO nanorod array-coated mesh films[J]. J. Mater. Chem., 2012, 22(37):19652-19657.
[14]ZHAOL,LIL,WANGY,etal.Preparationandcharacterization of thermo-andpHdual-responsive3Dcellulose-basedaerogelfor oil/water separation[J]. Appl. Phys. A:Mater., 2018, 124:9.
[15]CHEH,HUOM,PENGL,etal.CO2-responsivenanofibrous membraneswithswitchableoil/waterwettability[J].Angew.Chem.Int. Ed., 2015, 54:8934-8938.
[16]王金渠,杨建华,李华征,等.沸石分子筛膜研究进展[J].膜科学与技术, 2014, 34(3):1-7.WANG Jinqu, YANG Jianhua, LI Huazheng, et al. Advance in zeolite membrane research[J]. Membr. Sci. Techno., 2014, 34(3):1-7.
[17]李羚,朱美华,刘永生,等.耐酸性分子筛膜的研究进展[J].江西师范大学学报(自然科学版), 2017, 41(1):79-83.LILing,ZHUMeihua,LIUYongsheng,etal.Theresearch developmentoftheacid-resistantzeolitemembrane[J].J.Jiangxi Normal Univ.(Natural Science), 2017, 41(1):79-83.
[18]杨振生,李亮,张磊,等.疏水性油水分离膜及其过程研究进展[J].化工进展, 2014, 33(11):3082-3089.YANGZhensheng,LILiang,ZHANGLei,etal.Progressof hydrophobic membrane and process for oil/water separation[J]. Chem.Ind. Eng. Prog., 2014, 33(11):3082-3089.
[19]袁腾,陈卓,周显宏,等.基于超亲水超疏油原理的网膜及其在油水分离中的应用[J].化工学报, 2014, 65(6):1943-1951.YUAN Teng, CHEN Zhuo, ZHOU Xianhong, et al. Coated mesh film basedonsuperhydrophilicandsuperoleophobicprincipleandits applicationinoil-waterseparation[J].CIESCJournal,2014,65(6):1943-1951.
[20]江雷,邓琳.仿生智能纳米界面材料[M].北京:化学工业出版社,2007.JIANG Lei, DENG Lin. Bionic intelligent nano-interface material[M].Beijing:Chemical Industry Press, 2007.
[21]WOODWARDJT,GWINH,SCHWARTZDK.Contactangles on surfaces with mesoscopic chemical heterogeneity[J]. Langmuir, 2000,16(6):2957-2961.
[22]ERBILHY,DEMIRELAL,AVCIY,etal.Transformationofa simpleplasticintoasuperhydrophobicsurface[J].Science,2003,299(5611):1377-1380.
[23]VOGLEREA.Structureandreactivityofwateratbiomaterial surfaces[J]. Adv. Colloid Interface Sci., 1998, 74:69-117.
[24]ZHANG W, LIU N, CAO Y. et al. Superwetting porous materials for wastewater treatment:from immiscible oil/water mixture to emulsion separation[J]. Adv. Mater. Interfaces, 2017, 4(10):1700029.
[25]MIWAM,NAKAJIMAA,FUJISHIMAA,etal.Effectsofthe surfaceroughnessonslidinganglesofwaterdropletson superhydrophobic surfaces[J]. Langmuir, 2000, 16:5754-5760.
[26]CUIJ,ZHANGX,LIUH,etal.Preparationandapplicationof zeolite/ceramicmicrofiltrationmembranesfortreatmentofoil contaminated water[J]. J. Membr. Sci., 2008, 325(1):420-426.
[27]SCHEIBLERJR,SANTOSERF,BARBOSAAS,etal.Performanceofzeolitemembrane(ZSM-5/γ-Alumina)inthe oil/waterseparationprocess[J].Desalin.WaterTreat.,2015,56(13):3561-3567.
[28]WEN Q, DI J, JIANG L, et al. Zeolite-coated mesh film for efficient oil–water separation[J]. Chem. Sci., 2013, 4:591-595.
[29]ZENG J, GUO Z. Superhydrophilic and underwater superoleophobic MFI zeolite-coated film for oil/water separation[J]. Colloids Surf. A,2014, 444:283-288.
[30]LIUR,DANGWALS,SHAIKI,etal.Hydrophilicity-controlled MFI-typezeolite-coatedmesh for oil/waterseparation[J].Sep.Purif.Technol., 2018, 195:163-169.
[31]于吉红,温强,邸建城,等.一种无机相分离膜及其在油水分离中的应用:CN201210086896.0[P]. 2012-03-29.YUJihong,WENQiang,DIJiancheng,etal.Inorganicphase separation membrane and application thereof in oil-water separation:CN201210086896.0[P]. 2012-03-29.
[32]ZHANGF,ZHANGWB,SHIZ,etal.Nanowire-hairedinorganic membraneswithsuperhydrophilicityandunderwaterultralow adhesivesuperoleophobicityforhigh-efficiencyoil/waterseparation[J]. Adv. Mater., 2013, 2:4192-4198.
[33]LIU N, CHEN Y, LU F, et al. Straightforward oxidation of a copper substrate produces an underwater superoleophobic mesh for oil/water separation[J]. Chem. Phys. Chem., 2013, 14(15):3489-3494.
[34]WANG K, HAN D S, YIMING W, et al. A windable and stretchable three-dimensionalall-inorganicmembraneforefficientoil/water Separation[J]. Sci. Rep., 2017, 7:16081.
[35]LIJ,YANL,HUW,etal.Facilefabricationofunderwater superoleophobicTi O2coatedmeshforhighlyefficientoil/water separation[J]. Colloids Surf. A, 2016, 489:441-446.
[36]LIUN,LINX,ZHANGW,etal.ApureinorganicZnO-Co3O4overlapped membrane for efficient oil/water emulsions separation[J].Sci. Rep., 2015, 5:9688.
[37]李方,孟蝶.氧化石墨烯:膜科学的机遇与挑战[J].膜科学与技术, 2015, 35(6):106-112.LIFang,MENGDie,Grapheneoxide:challengesandopportunities for membrane science[J]. Membr. Sci. Techno., 2015, 35(6):106-112.
[38]HUANGY,LIH,WANGL,etal.Ultrafiltrationmembraneswith structure-optimized graphene-oxide coatings for antifouling oil/water separation[J]. Adv. Mater. Interfaces, 2015, 2:1400433.
[39]DONGY,LIJ,SHIL,etal.Underwatersuperoleophobicgraphene oxidecoatedmeshesfortheseparationofoilandwater[J].Chem.Comm., 2014, 50:5586.
[40]AOC,YUANW,ZHAOJ,etal.Superhydrophilicgraphene oxide@electrospuncellulosenanofiberhybridmembranefor high-efficiency oil/water separation[J]. Carbohyd. Polym., 2017, 175:216-222.
[41]GE J, SHI L, WANG Y, et al. Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill[J]. Nature Nanotech.,2017, 12:434-441.
[42]QIUS,HOUL,LIUJ.High-fluxcontinuousoilspillcollectionby usingahydrophobic/oleophilicnanofibrouscontainer[J].RSCAdv.,2017, 7:19434-19438.
[43]LIJ,XUC,ZHANGY,etal.Gravity-directedseparationofboth immiscibleandemulsifiedoil/watermixturesutilizingcoconutshell layer[J]. J. Colloid Interface Sci., 2018, 211:233-242.
[44]LUD,ZHANGT,GUTIERREZL,etal.Influenceofsurface propertiesoffiltration-layermetaloxideonceramicmembrane foulingduringultrafiltrationofoil/wateremulsion[J].Environ.Sci.Technol., 2016, 50:4668-4674.
[45]ZHAOX,CHENW,SUY,etal.Hierarchicallyengineered membranesurfaceswithsuperiorantifoulingandself-cleaning properties[J]. J. Membr. Sci., 2013, 441:93-101.