针对水包油乳液难以分离的问题,采用简单便捷的共沉积法对乙酸纤维素(CA)膜进行改性,将没食子酸(GA)、聚乙烯亚胺(PEI)和铜离子共沉积在CA膜表面,制备了新型超亲水/水下超疏油CuSO4@GA@PEI@CA复合膜。通过扫描电子显微镜、能量色散谱仪、傅里叶变换红外光谱仪、X射线光电子能谱仪对复合膜的形貌结构和化学组成进行了表征。结果表明:通过增加表面粗糙度和表面能,CuSO4@GA@PEI@CA复合膜表现出良好的亲水性和水下超疏油性能,其水接触角和水下油接触角分别为26.7°和162.1°;复合膜可以分离6种水包油乳液,渗透通量保持在478.18~577.73L/(m2·h);复合膜具有良好的循环使用性能,分离10次后其渗透通量仍能保持91%以上。
To address the challenge of oil-in-water emulsion separation,the cellulose acetate (CA) membrane was modified using a straightforward and practical co-deposition technique,where gallic acid (GA),polyethyleneimine (PEI),and copper ions were co-deposited on the surface of the CA membrane to prepare a novel superhydrophilic/underwater superoleophobic CuSO4@GA@PEI@CA composite membrane.The morphology and chemical composition of the composite membrane were characterized by SEM,EDS,FT-IR,and XPS.The results showed that by increasing the surface roughness and surface energy,the CuSO4@GA@PEI@CA composite membrane exhibited excellent hydrophilicity and underwater superoleophobic properties,and its water contact angle and underwater oil contact angle were 26.7° and 162.1°,respectively.In addition,six oil-in-water emulsions were successfully separated by the composite membrane,and the flux remained between 478.18 and 577.73L/(m2·h).The composite membrane also had good recycling performance,and its permeation flux remained above 91% after 10 separation cycles.
[1] José M H,Canejo J P,Godinho M H.Oil/water mixtures and emulsions separation methods-an overview[J].Materials,2023,16(6):2503.
[2] Li X Y,Jin X,Wu Y J,et al.A comprehensive review of lignocellulosic biomass derived materials for water/oil separation[J].Science of the Total Environment,2023,876:162549.
[3] Sun X F,Feng S J,Zhang Z,et al.Preparation and properties of a silver particle-coated and 1-dodecanethiol-modified superhydrophobic melamine sponge for oil/water separation[J].Frontiers of Chemical Science and Engineering,2022,16(8):1237-1246.
[4] Samuel O,Othman M H D,Kamaludin R,et al.Treatment of oily wastewater using photocatalytic membrane reactors:a critical review[J].Journal of Environmental Chemical Engineering,2022,10(6):108539.
[5] Mekonnen M M,Hoekstra A Y.Four billion people facing severe water scarcity[J].Science Advances,2016,2(2):1500323.
[6] Wang X Y,Huang W Q,Li X F,et al.Superhydrophilic mixed matrix membranes by using strategy of internal and external coupling for oil-in-water emulsion separation[J].Journal of Water Process Engineering,2021,43:102276.
[7] Guha I F,Varanasi K K.Separating nanoscale emulsions:progress and challenges to date[J].Current Opinion in Colloid & Interface Science,2018,36:110-117.
[8] Feng S J,Zhao J F,Zhang P Y,et al.Superhydrophilic/underwater superoleophobic oil-in-water emulsion separation membrane modified by the co-deposition of polydopamine and chitosan-tripolyphosphate nanoparticles[J].Journal of Environmental Chemical Engineering,2022,10(3):107407.
[9] Sutrisna P D,Kurnia K A,Siagian U W R,et al.Membrane fouling and fouling mitigation in oil-water separation:a review[J].Journal of Environmental Chemical Engineering,2022,10(3):107532.
[10] Abd Halim N S,Wirzal M D H,Hizam S M,et al.Recent development on electrospun nanofiber membrane for produced water treatment:a review[J].Journal of Environmental Chemical Engineering,2021,9(1):104613.
[11] Chu Z L,Feng Y J,Seeger S.Oil/water separation with selective superantiwetting/superwetting surface materials[J].Angewandte Chemie-International Edition,2015,54(8):2328-2338.
[12] Wang R,Zhu L,Zhu X,et al.A super-hydrophilic and underwater super-oleophobic membrane with robust anti-fouling performance of high viscous crude oil for efficient oil/water separation[J].Colloids and Surfaces A-Physicochemical and Engineering Aspects,2023,658:130662.
[13] Zhu Y Z,Wang D,Jiang L,et al.Recent progress in developing advanced membranes for emulsified oil/water separation[J].Npg Asia Materials,2014,6:101.
[14] Chen C L,Weng D,Mahmood A,et al.Separation mechanism and construction of surfaces with special wettability for oil/water separation[J].ACS Applied Materials & Interfaces,2019,11(11):11006-11027.
[15] Qu F S,Cao A K,Yang Y,et al.Hierarchically superhydrophilic poly(vinylidene fluoride) membrane with self-cleaning fabricated by surface mineralization for stable separation of oily wastewater[J].Journal of Membrane Science,2021,640:119864.
[16] Cheng Q F,Li M Z,Zheng Y M,et al.Janus interface materials:superhydrophobic air/solid interface and superoleophobic water/solid interface inspired by a lotus leaf[J].Soft Matter,2011,7(13):5948-5951.
[17] Yu J C,Cao C Q,Pan Y X.Advances of adsorption and filtration techniques in separating highly viscous crude oil/water mixtures[J].Advanced Materials Interfaces,2021,8(16):2100061.
[18] Kang J H,Sheng J L,Xie J Q,et al.Tubular Cu(OH)2 arrays decorated with nanothorny Co-Ni bimetallic carbonate hydroxide supported on Cu foam:a 3D hierarchical core-shell efficient electrocatalyst for the oxygen evolution reaction[J].Journal of Materials Chemistry A,2018,6(21):10064-10073.
[19] Cheng X Q,Wang Z X,Guo J,et al.Designing multifunctional coatings for cost-effectively sustainable water remediation[J].ACS Sustainable Chemistry & Engineering,2018,6(2):1881-1890.
[20] Sileika T S,Barrett D G,Zhang R,et al.Colorless multifunctional coatings inspired by polyphenols found in tea,chocolate,and wine[J].Angewandte Chemie-International Edition,2013,52(41):10766-10770.
[21] Ejima H,Richardson J J,Liang K,et al.One-step assembly of coordination complexes for versatile film and particle engineering[J].Science,2013,341(6142):154-157.
[22] Markovic D,Zille A,Ribeiro A I,et al.Antibacterial bio-nanocomposite textile material produced from natural resources[J].Nanomaterials,2022,12(15):2539.
基金资助
国家自然科学基金(21777143)