| 喷涂辅助界面聚合制备聚乙烯基聚酰胺纳滤膜 |
| 作者:陈德鉴1, 史晓辉2, 况武3,5, 李莹4,陈响1, 姚之侃1, 张林1 |
| 单位: 1. 浙江大学 化学工程与生物工程学院, 膜与水处理教育部工程中心, 杭州 310058; 2. 西安航天华阳机电装备有限公司, 西安 710100;3. 北京碧水源膜科技有限公司, 北京 101407; 4. 浙江科技大学 环境与资源学院, 杭州 310023;5. 中国城乡控股集团有限公司, 武汉 430056 |
| 关键词: 聚乙烯微孔膜; 喷涂; 界面聚合; 聚酰胺纳滤膜 |
| DOI号: 10.16159/j.cnki.issn1007-8924.2026.01.008 |
| 分类号: TQ028.8 |
| 出版年,卷(期):页码: 2026,46(1):78-87 |
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摘要: |
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聚酰胺纳滤膜因其优异的分离性能而被广泛应用,但传统界面聚合法(CIP)制备聚酰胺纳滤膜时存在分离层结构难控、溶液利用率低等问题。本研究将喷涂技术与界面聚合技术结合,以聚乙烯微孔膜为支撑层制备聚乙烯基纳滤膜(PE-NF),并详细探讨了膜制备参数对膜结构与性能的影响。结果表明,采用喷涂辅助界面聚合可获得表面更平整、结构更均一的分离层;在优化条件下,膜对硫酸钠的截留率超过98%,水渗透通量约为72 L/(m2·h),显著高于CIP制备的纳滤膜[<50 L/(m2·h)]。喷涂辅助界面聚合制得的纳滤膜较低的交联度、较大的孔径以及强表面负电性,在确保其优异分离性能的同时,实现了水通量的提升。本研究验证了喷涂辅助界面聚合在聚酰胺分离层可控构筑中的可行性与优势,为界面反应调控及新型纳滤膜的制备提供了参考。 |
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Polyamide nanofiltration (NF) membranes have been widely applied due to their excellent separation performance. However, conventional interfacial polymerization (CIP) often suffers from poor controllability of the selective layer structure and low utilization efficiency of reactant solutions. In this study, a spray-assisted interfacial polymerization technique was developed by combining spray coating with interfacial polymerization, using a polyethylene microporous membrane as the support to fabricate polyethylene-based nanofiltration membranes (PE-NF). The effects of preparation parameters on the membrane structure and separation performance were systematically investigated. Results showed that the spray-assisted interfacial polymerization produced a smoother and more uniform polyamide layer. Under optimized conditions, the resulting membrane exhibited a Na2SO4 rejection of over 98% and a water permeate flux of approximately 72 L/(m2·h), significantly higher than that of the CIP-prepared membrane [<50 L/(m2·h)]. The spray-assisted membrane exhibited a lower crosslinking degree, larger effective pore size and strong surface negativity, which collectively contributed to its enhanced water flux while maintaining excellent separation selectivity. This study demonstrates the feasibility and advantages of spray-assisted interfacial polymerization for the controlled construction of polyamide separation layers, providing a useful reference for the design and fabrication of advanced nanofiltration membranes. |
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基金项目: |
| 国家重点研发计划项目(2023YFB3810900); 浙江省“领雁”计划项目(2023C03150); 浙江省基础公益研究计划项目(LZJWY22B070004) |
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作者简介: |
| 陈德鉴(2002-),男,浙江温州人,硕士研究生,主要从事膜材料制备及应用研究 |
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参考文献: |
| [1]Lu D, Yao Z K, Jiao L, et al. Separation mechanism, selectivity enhancement strategies and advanced materials for mono-/multivalent ion-selective nanofiltration membrane[J]. Adv Membr, 2022, 2: 100032. [2]Guo H, Li X H, Yang W L, et al. Nanofiltration for drinking water treatment: A review[J]. Front Chem Sci Eng, 2022, 16(5): 681-698. [3]Elimelech M, Phillip W A. The future of seawater desalination: Energy, technology, and the environment[J]. Science, 2011, 333(6043): 712-717. [4]陈伯志, 马悦, 李璐, 等. 面向垃圾渗滤液深度处理的抗污染纳滤膜应用研究[J]. 膜科学与技术, 2024, 44(2): 134-139. [5]Shirazi M M A, Dumée L F. Membrane distillation for sustainable wastewater treatment[J]. J Water Process Eng, 2022, 47: 102670. [6]Tang C Y, Kwon Y N, Leckie J O. Effect of membrane chemistry and coating layer on physiochemical properties of thin film composite polyamide RO and NF membranes Ⅱ. Membrane physiochemical properties and their dependence on polyamide and coating layers[J]. Desalination, 2009, 242:168-182. [7]Christy C, Vermant S. The state-of-the-art of filtration in recovery processes for biopharmaceutical production[J]. Desalination, 2002, 147: 1-4. [8]杜文林, 任凤伟. 高通量聚乙烯基反渗透膜制备[J]. 膜科学与技术, 2025, 45(2): 100-108. [9]Wang S, Wang Z Y, Xia J Z, et al. Polyethylene-supported nanofiltration membrane with in situ formed surface patterns of millimeter size in resisting fouling[J]. J Membr Sci, 2021, 620: 118830. [10]张翠苗, 杜文林, 卢彦斌, 等. 聚乙烯基材反渗透膜的制备及性能研究[J]. 膜科学与技术, 2024, 44(3): 57-66. [11]Dou P J, Xu N Y, Wen H, et al. Facile hydrophilization of polyethylene substrate by in situ polymerization of m-phenylenediamine for preparing high-performance polyamide reverse osmosis membrane[J]. J Membr Sci, 2023, 683: 121777. [12]Pang H Z, Jin X G, Wang J, et al. High temperature resistant polyamide thin film composite nanofiltration membrane based on polyethylene substrate[J]. J Membr Sci, 2025, 721: 123811. [13]杨皓程, 徐志康. 界面聚合与薄层复合膜:历史、现状与反思[J]. 高分子通报, 2025,38(4): 651-658. [14]Fan H Y, Zhu C Y, Xue Y R, et al. Green fabrication of polyamide nanofiltration membranes with ultra-low chemical consumption by vacuum filtration-spraying assisted interfacial polymerization[J]. Desalination, 2025, 596: 118334. [15]Liu G, Wei M J, Xu Z Q, et al. How monomer concentrations influence structures and separation performances of polyamide nanofiltration membranes?[J]. J Membr Sci, 2025, 733: 124334. [16]刘佳欢, 王建强, 刘富. 单体扩散控制界面聚合制备聚酰胺薄层复合纳滤膜研究进展[J]. 膜科学与技术, 2025, 45(4): 194-205. [17]Donnan F G. Theory of membrane equilibria and membrane potentials in the presence of non-dialysing electrolytes. A contribution to physical-chemical physiology[J]. J Membr Sci, 1995, 100(1): 45-55. [18]Karan S, Jiang Z, Livingston A G. Sub-10 nm polyamide nanofilms with ultrafast solvent transport for molecular separation[J]. Science, 2015, 348(6241): 1347-1351. [19]Cao X L, Guo J L, Cai J, et al. The encouraging improvement of polyamide nanofiltration membrane by cucurbituril-based host-guest chemistry[J]. AICHE J, 2020, 66(4): e16879. [20]Shao D D, Yang W J, Xiao H F, et al. Self-cleaning nanofiltration membranes by coordinated regulation of carbon quantum dots and polydopamine[J]. ACS Appl Mater Interfaces, 2020, 12(1): 580-590. [21]Qian Y, Li H, Lu J, et al. Inhibiting polyamide intrusion of thin film composite membranes: Strategies and environmental implications[J]. Environ Sci Technol, 2023, 57(29): 10860-10869. [22]Chen J J, Zhang J, Wu X L, et al. Accurately controlling the hierarchical nanostructure of polyamide membranes via electrostatic atomization-assisted interfacial polymerization[J]. J Mater Chem A, 2020, 8(18): 9160-9167. [23]Sun N, Dou P J, He H L, et al. Polyethylene separator supported TFC nanofiltration membranes for arsenate removal: Impact of hydrolysis[J]. Sep Purif Technol, 2026, 380: 135450. [24]Liu Y T, Liang H, Bai L M, et al. Modeling insights into the role of support layer in the enhanced separation performance and stability of nanofiltration membrane[J]. J Membr Sci, 2022, 658: 120681. [25]Liu L F, Huang X, Zhang X, et al. Modification of polyamide TFC nanofiltration membrane for improving separation and antifouling properties[J]. RSC Adv, 2018, 8(27): 15102-15110. [26]Ang M B M Y, Ji Y L, Huang S H, et al. A facile and versatile strategy for fabricating thin-film nanocomposite membranes with polydopamine-piperazine nanoparticles generated in situ[J]. J Membr Sci, 2019, 579: 79-89. [27]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. [28]Liu T Y, Chen D D, Gao F, et al. Polyethylene separator-supported nanofiltration membranes for desalination[J]. J Appl Polym Sci, 2024, 141(33): e55829. [29]Peng H W, Tang Q Q, Tang S H, et al. Surface modified polyamide nanofiltration membranes with high permeability and stability[J]. J Membr Sci, 2019, 592: 117386. [30]Tang Y J, Xu Z L, Xue S M, et al. Tailoring the polyester/polyamide backbone stiffness for the fabrication of high performance nanofiltration membrane[J]. J Membr Sci, 2017, 541: 483-491. [31]Zhu J Y, Yuan S S, Uliana A, et al. High-flux thin film composite membranes for nanofiltration mediated by a rapid co-deposition of polydopamine/piperazine[J]. J Membr Sci, 2018, 554: 97-108. [32]Yuan B B, Jiang C, Li P F, et al. Ultrathin polyamide membrane with decreased porosity designed for outstanding water-softening performance and superior antifouling properties[J]. ACS Appl Mater Interfaces, 2018, 10(49): 43057-43067. [33]Wang T Y, Qiblawey H, Judd S, et al. Fabrication of high flux nanofiltration membrane via hydrogen bonding based co-deposition of polydopamine with poly (vinyl alcohol) [J]. J Membr Sci, 2018, 552: 222-233. [34]Guo Y S, Mi Y F, Zhao F Y, et al. Zwitterions functionalized multi-walled carbon nanotubes/polyamide hybrid nanofiltration membranes for monovalent/divalent salts separation[J]. Sep Purif Technol, 2018, 206: 59-68. [35]Zhang X, Lyu Y, Yang H C, et al. Polyphenol coating as an interlayer for thin-film composite membranes with enhanced nanofiltration performance[J]. ACS Appl Mater Interfaces, 2016, 8(47): 32512-32519. [36]Ding H Z, Xie F, Wang Z Y, et al. 2D nanosheets optimized electrospray-assisted interfacial polymeri-zation polyamide membrane with excellent separation performance[J]. J Membr Sci, 2022, 647: 120308. |
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