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Recycling end-of-life reverse osmosis membranes for nanofiltration membranes via layer-by-layer assembly

Authors： CUI Junbo, CHEN Yingbo, ZHANG Yuanyuan

Units： School of?Materials?Science?and?Engineering, State Key?Laboratory of Separation Membranes and Membrane?Processes,?Tiangong?University,?Tianjin 300387, China

KeyWords： end-of-life reverse osmosis membranes; polyamide; recycle; layer-by-layer assembly; nanofiltration membranes

ClassificationCode：TQ028.8

year,volume(issue):pagination： 2023,43(4):44-53

Abstract：

To solve the problem of environmental pollution caused by waste reverse osmosis (RO) membranes, we proposed to remove the pollutants and polyamide layer on the surface of the waste RO membranes by using oxidant cleaning, and then use layer-by-layer self-assembly (LbL) method to convert and regenerate the waste membranes after oxidation cleaning into nanofiltration (NF) membranes. The effect of preparation parameters in the layer-by-layer self-assembly process on the separation performance of NF membrane was studied. The results showed that the LbL NF membrane R-A4 with 4.0 layers had the best performance when the regenerated ultrafiltration (UF) membrane was used as the basement membrane, the concentration of NaCl in the polyelectrolyte solution was 0.25 g/L, the concentration of cationic/anionic polyelectrolyte was 0.5 g/L, and the deposition time was 20/10 minutes. The pure water permeability of R-A4 was 55 L/(m2·h·MPa), and the rejection rates of divalent inorganic salts Na2SO4 and MgSO4 were 98.5% and 98.1% respectively. It showed excellent long-term working stability.

Funds：

天津市科技支撑计划重点项目（20YFZCSN00930）

AuthorIntro：

崔俊博（1994-），女，河南周口市人，硕士研究生，研究方向为废旧反渗透膜的回收再利用

Reference：

[1] Contreras-Martínez J, García-Payo C, Arribas P, et al. Recycled reverse osmosis membranes for forward osmosis technology[J]. Desalination, 2021, 519: 115312.
[2] Pu L, Xia Q, Wang Y, et al. Tailored nanofiltration membranes with enhanced permeability and antifouling performance towards leachate treatment[J]. Journal of Membrane Science, 2022, 658: 120730.
[3] Lawler W, Bradford-Hartke Z, Cran M J, et al. Towards new opportunities for reuse, recycling and disposal of used reverse osmosis membranes[J]. Desalination, 2012, 299: 103–112.
[4] Ng Z C, Chong C Y, Sunarya M H, et al. Reuse potential of spent RO membrane for NF and UF process[J]. Membrane and Water Treatment, 2020, 11(5): 323–331.
[5] Coutinho de Paula E, Amaral M C S. Extending the life-cycle of reverse osmosis membranes: A review[J]. Waste Management & Research: The Journal for a Sustainable Circular Economy, 2017, 35(5): 456–470.
[6] Ould Mohamedou E, Penate Suarez D B, Vince F, et al. New lives for old reverse osmosis (RO) membranes[J]. Desalination, 2010, 253(1–3): 62–70.
[7] Raval H D, Chauhan V R, Raval A H, et al. Rejuvenation of discarded RO membrane for new applications[J]. Desalination and Water Treatment, 2012, 48(1–3): 349–359.
[8] Lawler W, Antony A, Cran M, et al. Production and characterisation of UF membranes by chemical conversion of used RO membranes[J]. Journal of Membrane Science, 2013, 447: 203–211.
[9] Veza J M, Rodriguez-Gonzalez J J. Second use for old reverse osmosis membranes: wastewater treatment[J]. Desalination, 2003, 157(1–3): 65–72.
[10] 祝文哲, 陈逸琛, 代丹阳, 等. 基于专家调查的我国旧RO膜回收利用及废弃膜处置市场研究[J]. 膜科学与技术, 2022, 3(42): 180-186,194.
[11] Zhang C, Ou Y, Lei W-X, et al. CuSO 4 /H 2 O 2 -Induced Rapid Deposition of Polydopamine Coatings with High Uniformity and Enhanced Stability[J]. Angewandte Chemie International Edition, 2016, 55(9): 3054–3057.
[12] Liu Y, Zheng S, Gu P, et al. Graphene-polyelectrolyte multilayer membranes with tunable structure and internal charge[J]. Carbon, 2020, 160: 219–227.
[13] Elshof M G, de Vos W M, de Grooth J, et al. On the long-term pH stability of polyelectrolyte multilayer nanofiltration membranes[J]. Journal of Membrane Science, 2020, 615: 118532.
[14] Ettori A. Permeability and chemical analysis of aromatic polyamide based membranes exposed to sodium hypochlorite[J]. Journal of Membrane Science, 2011, 375: 220–230.
[15] Steitz R, Jaeger W, Klitzing R v. Influence of Charge Density and Ionic Strength on the Multilayer Formation of Strong Polyelectrolytes[J]. Langmuir, 2001, 17(15): 4471–4474.
[16] Rojas O J, Claesson P M, Muller D, et al. The Effect of Salt Concentration on Adsorption of Low-Charge-Density Polyelectrolytes and Interactions between Polyelectrolyte-Coated Surfaces[J]. Journal of Colloid and Interface Science, 1998, 205(1): 77–88.
[17] Sun Q, Tong Z, Wang C, et al. Charge density threshold for LbL self-assembly and small molecule diffusion in polyelectrolyte multilayer films[J]. Polymer, 2005, 46(13): 4958–4966.
[18] Schoeler B, Kumaraswamy G, Caruso F. Investigation of the Influence of Polyelectrolyte Charge Density on the Growth of Multilayer Thin Films Prepared by the Layer-by-Layer Technique[J]. Macromolecules, 2002, 35(3): 889–897.
[19] Chen Y, Liu F, Wang Y, et al. A tight nanofiltration membrane with multi-charged nanofilms for high rejection to concentrated salts[J]. Journal of Membrane Science, 2017, 537: 407–415.
[20] Meng F, Song F, Yao Y, et al. Ultrastable Nanofiltration Membranes Engineered by Polydopamine-Assisted Polyelectrolyte Layer-by-Layer Assembly for Water Reclamation[J]. ACS Sustainable Chemistry & Engineering, 2020, 8(29): 10928–10938.
[21] Li X, Liu C, Yin W, et al. Design and development of layer-by-layer based low-pressure antifouling nanofiltration membrane used for water reclamation[J]. Journal of Membrane Science, 2019, 584: 309–323.
[22] Wang J, Zhu J, Tsehaye M T, et al. High flux electroneutral loose nanofiltration membranes based on rapid deposition of polydopamine/polyethyleneimine[J]. Journal of Materials Chemistry A, 2017, 5(28): 14847–14857.
[23] Wang H, Wei Z, Wang H, et al. An acid-stable positively charged polysulfonamide nanofiltration membrane prepared by interfacial polymerization of polyallylamine and 1,3-benzenedisulfonyl chloride for water treatment[J]. RSC Advances, 2019, 9(4): 2042–2054.
[24] 魏桐, 苏保卫, 高学理, 等. 基于配位作用的层层自组装正渗透膜及其制备方法[J]. 膜科学与技术, 2015, 35(5): 35–41.
[25] Chew N G P, Zhao S, Malde C, et al. Superoleophobic surface modification for robust membrane distillation performance[J]. Journal of Membrane Science, 2017, 541: 162–173.
[26] Liu C, Fang W, Chou S, et al. Fabrication of layer-by-layer assembled FO hollow fiber membranes and their performances using low concentration draw solutions[J]. Desalination, 2013, 308: 147–153.
[27] Simon A, Nghiem L D, Le-Clech P, et al. Effects of membrane degradation on the removal of pharmaceutically active compounds (PhACs) by NF/RO filtration processes[J]. Journal of Membrane Science, 2009, 340(1–2): 16–25.
[28] Do V T, Tang C Y, Reinhard M, et al. Degradation of Polyamide Nanofiltration and Reverse Osmosis Membranes by Hypochlorite[J]. Environmental Science & Technology, 2012, 46(2): 852–859.
[29] Choi J, Rubner M F. Influence of the Degree of Ionization on Weak Polyelectrolyte Multilayer Assembly[J]. Macromolecules, 2005, 38(1): 116–124.
[30] de Vos W M, Mears L L E, Richardson R M, et al. Nonuniform Hydration and Odd–Even Effects in Polyelectrolyte Multilayers under a Confining Pressure[J]. Macromolecules, 2013, 46(3): 1027–1034.
[31] Schlenoff J B, Dubas S T. Mechanism of Polyelectrolyte Multilayer Growth: Charge Overcompensation and Distribution[J]. Macromolecules, 2001, 34(3): 592–598.
[32] Liu C, Shi L, Wang R. Crosslinked layer-by-layer polyelectrolyte nanofiltration hollow fiber membrane for low-pressure water softening with the presence of SO 4 2− in feed water[J]. Journal of Membrane Science, 2015, 486: 169–176.
[33] Guo H, Ma Y, Sun P, et al. Self-cleaning and antifouling nanofiltration membranes—superhydrophilic multilayered polyelectrolyte/CSH composite films towards rejection of dyes[J]. RSC Advances, 2015, 5(78): 63429–63438.
[34] 苑宏英, 乔红伟, 韩嘉伟, 等. 纳滤膜对不同阴阳离子的截留效果及分析[J]. 环境科学与资源利用, 2019, 28(6): 408–412.
[35] Ding J, Wu H, Wu P. Preparation of highly permeable loose nanofiltration membranes using sulfonated polyethylenimine for effective dye/salt fractionation[J]. Chemical Engineering Journal, 2020, 396: 125199.
[36] Tansel B, Sager J, Rector T, et al. Significance of hydrated radius and hydration shells on ionic permeability during nanofiltration in dead end and cross flow modes[J]. Separation and Purification Technology, 2006, 51(1): 40–47.
[37] E. R N. Phenomenological theory of ion solvation. Effective radii of hydrated ions[J]. The Journal of Physical Chemistry, 1959(63): 1381–1387.
[38] Xu S, He R, Dong C, et al. Acid stable layer-by-layer nanofiltration membranes for phosphoric acid purification[J]. Journal of Membrane Science, 2022, 644: 120090.
[39] Lourenço J M C, Ribeiro P A, Botelho do Rego A M, et al. Counterions in Poly(allylamine hydrochloride) and Poly(styrene sulfonate) Layer-by-Layer Films[J]. Langmuir, 2004, 20(19): 8103–8109.
[40] Schönhoff M, Ball V, Bausch A R, et al. Hydration and internal properties of polyelectrolyte multilayers[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2007, 303(1–2): 14–29.
[41] Ghostine R A, Markarian M Z, Schlenoff J B. Asymmetric Growth in Polyelectrolyte Multilayers[J]. Journal of the American Chemical Society, 2013, 135(20): 7636–7646.
[42] Ang M B M Y, Ji Y-L, Huang S-H, et al. Incorporation of carboxylic monoamines into thin-film composite polyamide membranes to enhance nanofiltration performance[J]. Journal of Membrane Science, 2017, 539: 52–64.
[43] Ye C-C, Zhao F-Y, Wu J-K, et al. Sulfated polyelectrolyte complex nanoparticles structured nanoflitration membrane for dye desalination[J]. Chemical Engineering Journal, 2017, 307: 526–536.
[44] Zhao Q, An Q F, Ji Y, et al. Polyelectrolyte complex membranes for pervaporation, nanofiltration and fuel cell applications[J]. Journal of Membrane Science, 2011, 379(1–2): 19–45.
[45] Zhao Q, An Q, Sun Z, et al. Studies on Structures and Ultrahigh Permeability of Novel Polyelectrolyte Complex Membranes[J]. The Journal of Physical Chemistry B, 2010, 114(24): 8100–8106.

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