Investigation on Amino-Induced In-Situ Interfacial Copolymeri-zation Nanofiltration Membranes for Dye-Containing Wastewater Separation

Authors

  • Si Zhang "State Key Laboratory of Advanced Separation Membrane Materials, Tiangong University, Tianjin 300387, China" & "School of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China"
  • Hao Zhang State Key Laboratory of Advanced Separation Membrane Materials, Tiangong University, Tianjin 300387, China
  • Zhenjie Gu "State Key Laboratory of Advanced Separation Membrane Materials, Tiangong University, Tianjin 300387, China" & "School of Physical Science and Technology, Tiangong University, Tianjin 300387, China"
  • Zhihua Qiao "State Key Laboratory of Advanced Separation Membrane Materials, Tiangong University, Tianjin 300387, China" & "School of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China"

DOI:

https://doi.org/10.12974/2311-8717.2026.14.03

Keywords:

Textile wastewater, Nanofiltration membrane, Metal-organic framework, UiO-66-NH2, Interfacial polymerization, Dye rejection

Abstract

To address the demand for efficient dye separation and salt recovery in textile wastewater treatment, this study proposes a fabrication strategy for composite nanofiltration (NF) membranes modified with UiO-66-NH2. This approach involves introducing varying proportions of UiO-66-NH2 into the aqueous phase solution during interfacial polymerization. By leveraging the abundant amino active sites on the UiO-66-NH2 to undergo covalent reactions with acyl chloride monomers in the organic phase, in-situ chemical bonding between the MOF material and the polyamide (PA) separation layer was achieved concurrently with the interfacial polymerization of piperazine (PIP) and trimesoyl chloride (TMC). This method significantly enhanced the interfacial compatibility between the MOF nanoparticles and the polymer matrix, successfully yielding a series of thin-film nanocomposite (TFN) membranes with robust interfacial bonding characteristics. The incorporation of UiO-66-NH2 markedly improved membrane permeability and optimized its rejection performance toward various dyes. At an optimal loading of 0.15 wt%, the pure water flux of the composite membrane reached 45.77 L·m-2·h-1, representing an increase of more than 80% compared with the pristine membrane (24.65 L·m-2·h-1). Meanwhile, rejection efficiencies for methyl blue (MeB) and congo red (CR) were as high as 98.0%, while methyl orange (MO) and methylene blue (MB) achieved rejections exceeding 75.0% (75.6% and 83%, respectively). The membrane also exhibited good operational stability during a 12 h continuous filtration test, maintaining a flux decline of less than 8.5% and dye rejection rates stably maintained above 98% (for CR) and 75% (for MO), respectively. UiO-66-NH2 was uniformly incorporated into the PA network and formed stable covalent bonds, which effectively regulated the physicochemical properties of the membrane surface and separation channels, thereby simultaneously enhancing the water flux and dye rejection efficiency. This study provided an effective approach for developing NF membranes with high water permeability, high retention rate, and good stability for dye wastewater treatment.

References

Wang Y, Dong Y, Shao J, Zhao Z, Zhai H. Study on Preparation of calcium-based modified coal gangue and its adsorption dye characteristics. Molecules 2024; 29: 2183. https://doi.org/10.3390/molecules29102183

Xia W, Wu Q, Huang R, Tao Y, Wang K, Wu S, Wang S, Wang M, Li Q. Activation of peroxymonosulfate by palygorskite supported Co-Fe for water treatment. RSC Adv 2023; 13: 12483. https://doi.org/10.1039/D2RA07948H

Feng J, Ran X, Wang L, Xiao B, Lei L, Zhu J, Liu Z, Xi X, Feng G, Dai Z, Li R. The synergistic effect of adsorption-photocatalysis for removal of organic pollutants on mesoporous Cu2V2O7/Cu3V2O8/g-C3N4 heterojunction. Int J Mol Sci 2022; 23: 14264. https://doi.org/10.3390/ijms232214264

Rouhollahi, M; Mohammadi, T; Mohammadi, M; Ahmadzadeh-Tofighy, M. Fabrication of nanocomposite membranes containing Ag/GO nanohybrid for phycocyanin concentration. Sci Rep 2024; 14: 2. https://doi.org/10.1038/s41598-024-73719-8

Zhao DL, Feng F, Shen L, Huang Z, Zhao Q, Lin H, Chung TS. Engineering metal-organic frameworks (MOFs) based thin-film nanocomposite (TFN) membranes for molecular separation. Chem Eng J 2023; 454: 140447. https://doi.org/10.1016/j.cej.2022.140447

Shen L, Cheng R, Yi M, Hung W, Japip S, Tian L, Zhang X, Jiang S, Li S, Wang Y. Polyamide-based membranes with structural homogeneity for ultrafast molecular sieving. Nat Commun 2022; 13: 500. https://doi.org/10.1038/s41467-022-28183-1

Wei S, Chen Y, Hu X, Wang C, Huang X, Liu D, Zhang Y. Monovalent/Divalent salts separation via thin film nanocomposite nanofiltration membrane containing aminated TiO2 nanoparticles. J Taiwan Inst Chem Eng 2020; 112: 169-179. https://doi.org/10.1016/j.jtice.2020.06.014

Zhang H, Lin B, Pan J, Qi Y, Shen J, Gao C, Van-der-Bruggen B. Carboxyl-functionalized graphene oxide polyamide nanofiltration membrane for desalination of dye solutions containing monovalent salt. J Mem Sci 2017; 539: 128-137. https://doi.org/10.1016/j.memsci.2017.05.075

Aljundi IH. Desalination characteristics of TFN-RO membrane incorporated with ZIF-8 nanoparticles. Desalination 2017; 420: 12-20. https://doi.org/10.1016/j.desal.2017.06.020

Li J, Xie Y, Cheng L, Li X, Liu F, Wang Z. Photo-Fenton reaction derived self-cleaning nanofiltration membrane with MOFs coordinated biopolymers for efficient dye/salt separation. Desalination 2023; 553: 116459. https://doi.org/10.1016/j.desal.2023.116459

Wu X, Yang L, Meng F, Shao W, Liu X, Li M. ZIF-8-incorporated thin-film nanocomposite (TFN) nanofiltration membranes: Importance of particle deposition methods on structure and performance. J Membr Sci 2021; 632: 119356. https://doi.org/10.1016/j.memsci.2021.119356

Wu M, Sun Y, Ji T, Yu K, Liu L, He Y, Yan J, Meng S, Hu W, Fan X, Du D, Liu Y. Fabrication of water-stable MOF-808 membrane for efficient salt/dye separation. J Membr Sci 2023; 686: 122023. https://doi.org/10.1016/j.memsci.2023.122023

Zhang X, Zhang Y, Wang T, Fan Z, Zhang G. A thin film nanocomposite membrane with pre-immobilized UiO-66-NH2 toward enhanced nanofiltration performance. RSC Adv 2019; 9: 24802. https://doi.org/10.1039/C9RA04714J

Liu L, Huang X, Zhang X, Li K, Ji Y, Yu C, Gao C. Modification of polyamide TFC nanofiltration membrane for improving separation and antifouling properties. RSC Adv 2018; 8: 15102-15110. https://doi.org/10.1039/C8RA01374H

Xiao F, Hu X, Chen Y, Zhang Y. Porous Zr-based metal organic frameworks (Zr-MOFs) incorporated thin-film nanocomposite membrane toward enhanced desalination performance. ACS Appl Mater Interfaces 2019; 11: 47390-47403. https://doi.org/10.1021/acsami.9b17212

Jiang C, Zhang M, Hou Y. Thin-Film Composite Membrane with Porous Interlayer Composed of Dendritic Mesoporous Silica Nanoparticles for Enhanced Nanofiltration. Polymers 2023; 15: 3912. https://doi.org/10.3390/polym15193912

Yu C, Cen X, Ao D, Qiao Z, Zhong C. Preparation of thin-film composite membranes with ultrahigh MOFs loading through polymer-template MOFs induction secondary interfacial polymerization. Appl Surf Sci 2023; 614: 156186. https://doi.org/10.1016/j.apsusc.2022.156186

Plisko T, Burts K, Zolotarev A, Bildyukevich A, Dmitrenko M, Kuzminova A, Ermakov S, Penkova A. Development and investigation of hierarchically structured thin-film nanocomposite membranes from polyamide/chitosan succinate embedded with a metal-organic framework (Fe-BTC) for pervaporation. Membranes 2022; 12: 967. https://doi.org/10.3390/membranes12100967

Song Z, Qiu F, Zaia EW, Wang Z, Kunz M, Guo J, Brady M, Mi B, Urban JJ. Dual-channel, molecular-sieving core/shell ZIF@MOF architectures as engineered fillers in hybrid membranes for highly selective CO2 separation. Nano Lett 2017; 17: 6752-6758. https://doi.org/10.1021/acs.nanolett.7b02910

Jia Y, Huo X, Gao L, Shao W, Chang N. Controllable design of polyamide composite membrane separation layer structures via metal-organic frameworks: a review. Membranes 2024; 14: 9. https://doi.org/10.3390/membranes14090201

Goh PS, Samavati Z, Ismail AF, Ng BC, Abdullah MS, Hilal N. Modification of liquid separation membranes using multidimensional nanomaterials: revealing the roles of dimension based on classical titanium dioxide. 2023; 13: 448. https://doi.org/10.3390/nano13030448

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Published

2026-04-02

How to Cite

Zhang, S. ., Zhang, H. ., Gu, Z. ., & Qiao, Z. . (2026). Investigation on Amino-Induced In-Situ Interfacial Copolymeri-zation Nanofiltration Membranes for Dye-Containing Wastewater Separation . Journal of Composites and Biodegradable Polymers, 14, 26–34. https://doi.org/10.12974/2311-8717.2026.14.03

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