PEI/SA/Cu三元体系改性荷正电纳滤膜及其脱盐性能
作者:马晓华, 梁晓康,许振良
单位: 华东理工大学,化工学院,化学工程研究所,膜科学与工程研发中心,上海 200237
关键词: PEI/SA/Cu三元体系改性;荷正电;纳滤膜;脱盐性能
DOI号:
分类号: TQ028.8
出版年,卷(期):页码: 2024,44(4):8-16

摘要:
?通过将海藻酸钠(SA)与聚乙烯亚胺(PEI)共混作为二次界面聚合反应的水相溶液,SA与PEI强相互作用使SA嵌入到聚酰胺层中,从而提高膜的致密性。随后通过Cu2+与SA结合提高膜表面荷正电性,提高膜对多价阳离子的截留性能。对比研究了SA和Cu2+浓度对复合膜物化性质、表面形貌及分离性能的影响。结果表明,荷正电纳滤膜的最佳制备条件为:SA质量分数为0.01 %,Cu2+浓度为25 mM,所对应的PS/Cu-3复合膜亲水性提高。与Control-PEI膜相比,其通量提高了257%,为(40.0 ± 0.8) L /(m2 h),对MgCl2的截留率从92.0%提升至97.1%,且具有良好的耐压性和稳定性。
 
 In this paper, sodium alginate (SA) and polyethylenimine (PEI) were blended as aqueous solution for secondary interfacial polymerization (SIP) reaction. The strong interaction between PEI and SA made SA embed into polyamide (PA) layer, thus improving the density of the membrane. Subsequently, the surface positive charge was improved through the complexation of Cu2+ with SA and PEI, and the retention of polyvalent cations was improved. The effects of SA and Cu2+ concentrations on physicochemical properties, surface morphology and separation performance of the composite membranes were studied. The results showed that the optimal membrane preparation conditions were as follows: SA concentration was 0.01 wt%, Cu2+ concentration was 25 mM. The corresponding PS/Cu-3 composite membrane has enhanced hydrophilicity and density, and decreased pore size. Compared with Control-PEI membrane, its flux is increased by 257% to 40.0 ± 0.8 L  /(m2 h), and the rejection of MgCl2 is increased from 92.0% to 97.1%, and it has good pressure resistance and stability.

基金项目:
国家重点研发计划项目(2021YFB3801103)

作者简介:
马晓华(1984—),女,四川南充人,教授,博士生导师,主要研究方向:分离膜制备与表征。

参考文献:
 [1] Gong X Y,Huang Z H,Zhang H, et al. Novel high-flux positively charged composite membrane incorporating titanium-based MOFs for heavy metal removal[J].Chem Eng J, 2020,398:125706.
[2] Li J P,Peng H W,Liu K K, et al. Polyester Nanofiltration Membranes for Efficient Cations Separation[J]. Adv Mater, 2024, 36(9):2309406.
[3] Peng H W,Zhao Q.A Nano-Heterogeneous Membrane for Efficient Separation of Lithium from High Magnesium/Lithium Ratio Brine[J]. Adv Funct Mater, 2021, 31(14):1-7.
[4] Xu P,Gonzales R R,Hong J, et al.Fabrication of highly positively charged nanofiltration membranes by novel interfacial polymerization: Accelerating Mg2+ removal and Li+ enrichment[J].J Membr Sci, 2023, 668:121251.
[5] Zhou Z Z,Lu T D,Sun S P, et al. Roles and gains of coordination chemistry in nanofiltration membrane: A review[J]. Chemosphere, 2023,318:137930.
[6] He J S,Wang Y,Ni F, et al. Ultra-Highly permeable loose nanofiltration membrane containing PG/PEI/Fe3+ ternary coating for efficient dye/salt separation[J]. Sep Purif Technol, 2022, 292: 121020.
[7] Yang Z,Zhou Z W,Guo H, et al. Tannic Acid/Fe3+ Nanoscaffold for Interfacial Polymerization: Toward Enhanced Nanofiltration Performance[J]. Environ Sci Technol, 2018,52(16): 9341-9349.
[8] Shao L P,Li Y,Pan F S, et al. Graphene oxide membranes tuned by metal-phytic acid coordination complex for butanol dehydration[J]. J Membr Sci, 2021, 638:119736.
[9] Xu J,Feng X S,Chen P P. Development of an antibacterial copper (II)-chelated polyacrylonitrile ultrafiltration membrane[J]. J Membr Sci, 2012, 413-414:62-69.
[10] Zhou T,Huang Y.Fe(III)EDTA and Fe(II)EDTA-NO reduction by supported (nano)ZVI in Fe(II)EDTA complexation denitrification technology: Performance, kinetics, and pathway[J]. J Environ Eng, 2022, 10(6):108547.
[11] Wang J,Liu S R,Mu Y N, et al.Sodium citrate complexing agent-dependent growth of n- and p-type CdTe thin films for applications in CdTe/CdS based photovoltaic devices[J]. J Alloy Compd, 2018, 748:515-521.
[12] Li X Y,Wang K K,Wang M Q, et al.Sustainable electrochemical dyeing of indigo with Fe(Ⅱ)-based complexes[J]. J Clean Prod, 2020,276:123251.
[13] Bechtold T,Burtscher E,Turcanu A.Ca2+–Fe3+–D-gluconate-complexes in alkaline solution. Complex stabilities and electrochemical properties[J]. Dalton T, 2002,2(13):2683-2688.
[14] Emam H E,Manian A P,Siroka B.Copper inclusion in cellulose using sodium D-gluconate complexes[J]. Carbohyd Polym, 2012,90(3):1345-1352.
[15] Metecan A,Cihano?lu A,Alsoy Altinkaya S.A positively charged loose nanofiltration membrane fabricated through complexing of alginate and polyethyleneimine with metal ions on the polyamideimide support for dye desalination[J]. Chem Eng J, 2021,416:128946.
[16] Gao X P,Guo C,Hao J J, et al. Adsorption of heavy metal ions by sodium alginate based adsorbent-a review and new perspectives[J]. Int J Biol Macromol, 2020,164: 4423-4434.
[17] Wu X Q, Song Y T,Yin P, et al. Fabrication of the composite sepiolite@polyethyleneimine/sodium alginate and its excellent adsorption performance for heavy metal ions[J]. Appl Clay Sci, 2022,228:106647.
[18] Zhu J H,Zheng J F,Liu C L, et al.Ionic complexing induced fabrication of highly permeable and selective polyacrylic acid complexed poly (arylene ether sulfone) nanofiltration membranes for water purification[J]. J Membr Sci, 2016,520:130-138.
[19] Khan S U,Sultan M,Islam A, et al.Sodium alginate blended membrane with polyurethane: Desalination performance and antimicrobial activity evaluation[J]. Int J Biol Macromol, 2021,182:72-81.
[20] Chen Y L,Feng J J,Fang M W, et al.Large-scale, ultrastrong Cu2+ cross-linked sodium alginate membrane for effective salinity gradient power conversion[J]. ACS Appl Polym Mater, 2021,3(8):3902-3910.
[21] Tekinalp O, Alsoy Altinkaya S. Development of high flux nanofiltration membranes through single bilayer polyethyleneimine/alginate deposition[J]. J Colloid Interface Sci, 2019,537: 215-227.
[22] Tang B B, Huo Z B,Wu P Y, et al.Study on a novel polyester composite nanofiltration membrane by interfacial polymerization of triethanolamine (TEOA) and trimesoyl chloride (TMC): I. Preparation,  characterization and nanofiltration properties test of membrane[J]. J Membr Sci, 2008, 320(1-2):198-205.
[23] Li Y H,Wang S H,Wu W Y, et al. Fabrication of positively charged nanofiltration membrane with uniform charge distribution by reversed interfacial polymerization for Mg2+/Li+ separation[J]. J Membr Sci, 2022,659:120809.
[24] Chen Y D,Sun R Z,Yan W T, et al.Antibacterial polyvinyl alcohol nanofiltration membrane incorporated with Cu(OH)2 nanowires for dye/salt wastewater treatment[J]. Sci Total Environ, 2022,817:152897.
[25] Xu J,Zhang L L,Gao X L, et al. Constructing antimicrobial membrane surfaces with polycation–copper(II) complex assembly for efficient seawater softening treatment[J]. J Membr Sci, 2015,491: 28-36.
[26] Luo J Q,Wan Y H. Mix-charged nanofiltration membrane: Engineering charge spatial distribution for highly selective separation[J]. Chem Eng J, 2023, 464:142689.
[27] Hejase C A,Tarabara V V.Nanofiltration of saline oil-water emulsions: combined and individual effects of salt concentration polarization and fouling by oil[J]. J Membr Sci, 2021, 617:118607.
[28] Xiang J,Li H,Hei Y H, et al. Preparation of highly permeable electropositive nanofiltration membranes using quaternized polyethyleneimine for dye wastewater treatment[J].J Water Process Eng, 2022, 48:102831.
[29] Fang L F,Zhou M Y,Cheng L, et al.Positively charged nanofiltration membrane based on cross-linked polyvinyl chloride copolymer[J]. J Membr Sci, 2019,572:28-37.
[30] Wu H H,Zhao H Y,Lin Y K, et al.Positively-charged PEI/TMC nanofiltration membrane prepared by adding a diamino-silane coupling agent for Li+/Mg2+ separation[J]. J Membr Sci, 2023,672: 121468.
[31] Xu P,Wang W,Qian X M, et al. Positive charged PEI-TMC composite nanofiltration membrane for separation of Li+ and Mg2+ from brine with high Mg2+/Li+ ratio[J]. Desalination, 2019, 449:57-68.
[32] Wang Z Y,Xie F,Ding H Z, et al. Effects of locations of cellulose nanofibers in membrane on the performance of positively charged membranes[J]. J Membr Sci, 2022,652:120464.
[33] Lin C E,Fang L F,Du S Y, et al.A novel positively charged nanofiltration membrane formed via simultaneous cross-linking/quaternization of poly( m -phenylene isophthalamide)/ polyethyleneimine blend membrane[J]. Sepa Purif Technol, 2019,212:101-109.
[34] Li T Y,Zhang X Z,Zhang Y, et al. Nanofiltration membrane comprising structural regulator Cyclen for efficient Li+/Mg2+ separation[J]. Desalination, 2023, 556:116575.
[35] Li H Y, Li Y H,Li M,et al. Improving Mg2+/Li+ separation performance of polyamide nanofiltration membrane by swelling-embedding-shrinking strategy[J]. J Membr Sci, 2023, 669: 121321.
 

服务与反馈:
文章下载】【加入收藏

《膜科学与技术》编辑部 地址:北京市朝阳区北三环东路19号蓝星大厦 邮政编码:100029 电话:010-64426130/64433466 传真:010-80485372邮箱:mkxyjs@163.com

京公网安备11011302000819号