Vapor/Vapor-Solid Interfacial Growth of Covalent Organic Framework Membranes on Alumina Hollow Fiber for Advanced Molecular Separation.

Covalent organic frameworks (COFs), known for their chemical stability and porous crystalline structure, hold promises as advanced separation membranes. However, fabricating high-quality COF membranes, particularly on industrial-preferred hollow fiber substrates, remains challenging. This study introduces a novel vapor/vapor-solid (V/V-S) method for growing ultrathin crystalline TpPa-1 COF membranes on the inner lumen surface of alumina hollow fibers (TpPa-1/Alumina). Through vapor-phase monomer introduction onto polydopamine-modified alumina at 170 °C and 1 atm, efficient polymerization and crystallization occur at the confined V-S interface. This enables one-step growth within 8 h, producing 100 nm thick COF membranes with strong substrate adhesion. TpPa-1/Alumina exhibits exceptional stability and performance over 80 h in continuous cross-flow organic solvent nanofiltration (OSN), with methanol permeance of about 200 L m-2 h-1 bar-1 and dye rejection with molecular weight cutoff (MWCO) of approximately 700 Da. Moreover, the versatile V/V-S method synthesizes two additional COF membranes (TpPa2Cl/Alumina and TpHz/Alumina) with different pore sizes and chemical environments. Adjusting the COF membrane thickness between 100-500 nm is achievable easily by varying the growth cycle numbers. Notably, TpPa2Cl/Alumina demonstrates excellent OSN performance in separating the model active pharmaceutical ingredient glycyrrhizic acid (GA) from dimethyl sulfoxide (DMSO), highlighting the method's potential for large-scale industrial applications.

Recycling the High-Salinity Textile Wastewater by Quercetin-Based Nanofiltration Membranes with Minimal Water and Energy Consumption.

Effective recovery of dyes and salts from textile wastewater by nanofiltration (NF) remains a serious challenge due to the high consumption of water and energy caused by the limited performance of the available membranes. Herein, a novel strategy is described to prepare loose polyester NF membranes by using renewable quercetin as the aqueous monomer for fractionation of high salinity textile wastewater with minimal water and energy consumption. Compared with NF270, taken as the reference membrane, the QE-0.2/TMC-0.2 membrane significantly improved the efficiency for dye/salt fractionation by 288%. The water consumption was also decreased by 42.9%. The efficiency is attributed to an ultrahigh water permeance of 198 ± 2.1 L-1 m-2 h-1 bar-1 with a high selectivity of 123 (extremely low NaCl rejection of 1.6% and high Congo red rejection of 99.2%). The optimal quercetin-based membrane had an ultrathin separation layer of about 39 ± 1.2 nm with good hydrophilicity and negative charge density. Moreover, this work includes a novel method of comparison with a theoretically ideal membrane, which shows that both the energy and water consumption are near their theoretical minimum. This strategy is expected to save energy and minimize carbon emissions for membrane-based wastewater treatment systems.

Energy-efficient trehalose-based polyester nanofiltration membranes for zero-discharge textile wastewater treatment.

Recovery of water, salts, and hazardous dye from complex saline textile wastewater faces obstacles in separating dissolved ionic substances and recovering organic components during desalination. This study realized the simultaneous fractionation, desalination, and dye removal/recovery treatment of textile wastewater by using trehalose (Tre) as an aqueous monomer to prepare polyester loose nanofiltration (LNF) membrane with fine control microstructure via interfacial polymerization. Outperforming the NF270 commercial membrane, the Tre-1.05/TMC optimized membrane achieves zero-discharge textile wastewater treatment, cutting energy consumption by 295% and reducing water consumption by 42.8%. This efficiency surge results from remarkable water permeability (130.83 L m-2 h-1 bar-1) and impressive dye desalination (NaCl/ Direct Red 23 separation factor of 275) of the Tre-1.05/TMC membrane. For a deeper comprehension of filtration performance, the sieving mechanism of polyester LNF membranes was systematically elucidated. This strategic approach offers significant prospects for energy conservation, carbon emission mitigation, and enhanced feasibility of membrane-based wastewater treatment systems.

Low Fouling Polyelectrolyte Layer-by-Layer Self-Assembled Membrane for High Performance Dye/Salt Fractionation: Sequence Effect of Self-Assembly.

Layer-by-layer (LbL) self-assembly of oppositely charged polyelectrolytes (PEs) is usually performed on a conventional ultrafiltration base substrate (negative zeta potential) by depositing a cationic PE as a first layer. Herein, we report the facile and fast formation of high performance molecular selective membrane by the nonelectrostatic adsorption of anionic PE on the polyvinylidene fluoride (PVDF, zeta potential -17 mV) substrate followed by the electrostatic LbL assembly. Loose nanofiltration membranes have been prepared via both concentration-polarization (CP-LbL, under applied pressure) driven and conventional (C-LbL, dipping) LbL self-assembly. When the first layer is poly(styrene sodium) sulfonic acid, the LbL assembled membrane contains free -SO3- groups and exhibits higher rejection of Na2SO4 and lower rejection of MgCl2. The reversal of salt rejection occurs when the first layer is quaternized polyvinyl imidazole (PVIm-Me). The membrane (five layers) prepared by first depositing PStSO3Na shows higher rejection of several dyes (97.9 to >99.9%), higher NaCl to dye separation factor (52-1800), and higher dye antifouling performance as compared to the membrane prepared by first depositing PVIm-Me (97.5-99.5% dye rejection, separation factor ∼40-200). However, the C-LbL membrane requires a longer time of self-assembly or higher PE concentration to reach a performance close to the CP-LbL membranes. The membranes exhibit excellent pressure, pH (3-12), and salt (60 g L-1) stability. This work provides an insight for the construction of low fouling and high-performance membranes for the fractionation of dye and salt based on the LbL self-assembly sequence.

Fabrication of hollow fiber composite membranes via opposite transmission reaction method for dye/salt separation.

The separation layer prepared by the conventional coating-crosslinking method is typically thick and prone to forming defective macropores, significantly affecting the water permeability and dye/salt separation performance of membranes. This work presented a novel method to prepare hollow fiber composite membranes for dye/salt separation based on the opposite transmission reaction of crosslinker. In this method, the macromolecule in situ reacted with a small-molecule crosslinker at the openings of membrane pore channels, forming a separation layer with discontinuous sheet-like and granular structure. Compared to the conventional forward coating-crosslinking method, the separation layer prepared by the opposite transmission reaction method exhibited an ultra-thin thickness of 29.1 nm. Consequently, the composite membrane exhibited a high water permeability of 72.7 L·m-2·h-1·bar-1, which was 2.3 times higher than that of conventional methods. Moreover, the prepared composite membrane presented a more uniformed pore structure, completely retaining the VBB (100%) with a low Na2SO4 rejection of 4.3%, demonstrating excellent dye/salt separation performance. Additionally, the prepared composite membrane exhibited superior anti-fouling properties compared to that prepared by the conventional method. Therefore, the opposite transmission reaction method proposed in this study held promising applications in the preparation of hollow fiber composite membranes for efficient dye/salt separation.

Cellulose acetate, a source from discarded cigarette butts for the development of mixed matrix loose nanofiltration membranes for selective separation.

This study presents an environmentally friendly method for extracting cellulose acetate (CA) from discarded cigarette filters, which is then utilized in the fabrication of cellulose-based membranes designed for high flux and rejection rates. CA membranes are likeable to separate dyes and ions, but their separation efficiency is exposed when the contaminant concentration is very low. So, we have integrated graphene oxide (GO) and carboxylated titanium dioxide (COOH-TiO2) in CA to develop mixed matrix membranes (MMMs) and studied them against dyes and most used salts. The CA has been extracted from these butts and added GO and COOH-TiO2 nanoparticles to develop MMMs. The present work administers the effective separation of five dyes (methyl orange, methyl violet, methylene blue, cresol red, and malachite green) and salts (NaCl and Na2SO4) along with the high efficiency of water flux by prepared CA membranes. The prepared membranes rejected up to 94.94 % methyl violet, 91.28 % methyl orange, 88.28 % methylene blue, 89.91 % cresol red, and 91.70 % malachite green dye. Along with the dyes, the membranes showed ∼40.40 % and âˆ¼ 42.97 % rejection of NaCl and Na2SO4 salts, respectively. Additionally, these membranes have tensile strength up to 1.54 MPa. Various characterization techniques were performed on all prepared CA membranes to comprehend their behaviour. The antibacterial activity of MMMs was investigated using the Muller-Hinton-Disk diffusion method against the gram-positive bacterium Staphylococcus aureus (S. aureus) and the gram-negative bacterium Escherichia coli (E. coli). We believe the present work is an approach to utilizing waste materials into valuable products for environmental care.

Loose Nanofiltration Membrane Incorporating CeZnFe Layered Double Hydroxide with Enhanced Dye/Salt Separation Performance and Self-Cleaning Ability.

The high-salinity wastewater from the textile industry faces a significant challenge in effectively separating dyes and salts. In this study, a CeZnFe-layered double hydroxide (LDH)-incorporated nanofiltration (LNF) membrane was fabricated using the conventional interfacial polymerization (IP) technique to fractionate dyes and salts within the wastewater. The impact of CeZnFe LDH on various aspects of membrane performance was examined, including water flux, dye removal efficiency, dye/salt separation capability, self-cleaning ability, and membrane integrity. The addition of LDHs resulted in improved membrane surface hydrophilicity, thereby enhancing water flux. The optimized TFN membrane (0.050 wt% LDH in PIP solution) significantly improved pure water flux, exceeding 150%. All TFN membranes exhibited excellent performance in dye and salt fractionation (93% for Congo red, 2.6% for NaCl, and 40.7% for Na2SO4). Also, excellent self-cleaning ability was observed for the optimized membrane, exhibiting a remarkable water flux recovery rate after three operation cycles. Moreover, including CeZnFe LDH in the optimized TFN membrane played a significant role in enhancing membrane integrity. This study provides new inspiration for fabricating self-cleaning loose NF membranes using CeZnFe LDH for effective dye/salt separation.

Interfacial Polymerization of Highly Active Thiolated Cyclodextrin for the Fabrication of a Loose Nanofiltration Membrane with a Chlorine-Resistant Poly(thioester) Linkage.

Cyclodextrins have been frequently used to fabricate membranes via interfacial polymerization (IP). However, the relatively low reactivity of pristine cyclodextrins often induces a lower cross-linking density and unsatisfactory separation performance. In this work, to introduce a highly active thiolated ß-cyclodextrin (CD-SH) monomer into IP progress, we constructed a dense and porous poly(thioester) linkage on a commercial membrane surface with loose nanofiltration by IP of CD-SH and trimesoyl trichloride (TMC) as the monomer in an aqueous phase and organic phase separately for the first time. Furthermore, the reactivity of CD-SH has been fully demonstrated by the two-phase IP aiming at unmodified ß-CD, a CD-SH/TMC freestanding membrane with a thicker interfacial layer and a smoother surface, and a PAN/CD-SH membrane with a narrow porous distribution. The composite membrane possessed superior separation performance for a high rejection (83.1-99.6%) of different anionic dyes and a low rejection (<20%) of salts, as well as a high-efficiency sieving ability of dye/dye and dye/salt mixtures. The membrane with a poly(thioester) selective layer could steadily operate in a long-term filtration test and exhibit great stability, chloride-resistance performance, and recyclability.

Application of moving bed biofilm reactor - nanofiltration - membrane bioreactor with loose nanofiltration hollow fiber membranes for synthetic roxithromycin-containing wastewater treatment: Long-term performance, membrane fouling and microbial community.

The present study operated the novel moving bed biofilm reactor-nanofiltration-membrane bioreactor (MBBR-NF-MBR) with loose polyamide NF membranes for the first time to treat roxithromycin (ROX) wastewater. Results showed that both MBBR-NF-MBRs achieved superior COD removal of 98.4% and 97.2% and excellent removal of ROX at 74.1% and 65.5%, respectively. The main membrane fouling mechanism was reversible fouling caused by the combination of abundant polysaccharides, proteins and Ca-P precipitates, which could be effectively removed by acidic cleaning. Sorption and biodegradation were the main removal routes of ROX in MBBR. Partial retention of loose NF membrane contributed to microbial metabolism and increased microbial diversity, especially the genera Hyphomicrobium in attached biofilm, which was reasonable for ROX removal. The cleavage of cladinose, demethylation, phosphorylation and ß-oxidation in macrolactone ring were the main biotransformation reactions of ROX. This study provides novel insights for micropollutants wastewater treatment by using loose NF membrane in MBR.

Design of microstructure for hollow fiber loose nanofiltration separation layer and its compactness-tailoring mechanism.

In order to promote the application of membrane technology in the treatment of textile wastewater containing small molecule dye, fabricating a hollow fiber loose nanofiltration (LNF) with a thin and compact separation layer and deepening the understanding of compactness-tailoring mechanism in chemical crosslinking are essential. Firstly, the mechanisms of synergistic crosslinking of PEI-70K and PEI-10K, along with a weakening of the PEI hydration by ethanol, were expounded in primary crosslinking. Then, some LNF separation layers with different compactness were prepared through crosslinking with different crosslinkers to further reduce pore size, which resulted in the efficient removal (~100%) of a small molecular dye (methyl orange (MO), M = 327 g mol-1). The removal of methyl orange is mainly caused by size sieving. The relationship among the pore size, the Mw of the secondary crosslinkers, and the pore size reduction rate was interpreted by comparing the pore size reduction rate of three secondary crosslinkers with different molecular weights. In addition, the as-prepared separation layer exhibited excellent dimensional stability and solvent resistance. This paper not only provides a reference for fabricating hollow fiber LNF with better purification performance, but also shows their potential in developing solvent resistant nanofiltration.

Low-pressure highly permeable polyester loose nanofiltration membranes tailored by natural carbohydrates for effective dye/salt fractionation.

With the continuous pressure of water contamination caused by textile industry, loose nanofiltration (LNF) membranes prepared by green materials with an extraordinary water permeability are highly desirable for the recovery and purification of dyes and salts. In this work, low-pressure LNF membranes with ultrahigh permeability were fabricated via one-step interfacial polymerization (IP), in which inexpensive natural carbohydrate-derived sugars with large size and low reactivity were utilized as aqueous monomers to design selective layer. A systematic characterization by chemical analysis and optical microscopy demonstrated that the formed polyester film features not only loosen the structure, but also results in a hydrophilic and negatively charged surface. The optimized sucrose-based membrane (Su0.6/TMC0.1) with an excellent water permeability of 52.4 LMH bar-1 was found to have a high rejection of dyes and a high transmission of salts. In addition, the sugar-based membrane manifested an excellent anti-fouling performance and long-term stability. Furthermore, the non-optimized Gl0.6/TMC0.1 and Ra0.6/TMC0.1 membranes also shown a high water permeability, while maintaining a competitive dye/salt separation performance, which confirmed the universal applicability of the membrane design principle. Therefore, the proposed new strategy for preparing next-generation LNF membranes can contribute towards the textile wastewater treatment.

Metal-polyphenol cross-linked titanium carbide membranes with stable interlayer spacing for efficient wastewater treatment.

Membranes based on transition metal carbides/nitrides (MXenes) have significant water treatment potential because of their unique molecular sieving properties and excellent permeation performance. However, hydrophilic MXenes swell upon water immersion, and improving their stability remains challenging. In this study, a Fe3+-tannic acid (TA) complex was used as a cross-linker and surface modifier to prepare high-performance titanium carbide (Ti3C2Tx) MXene laminar membranes. Fe3+-TA formation on the nanosheets increased the interlayer spacing and stabilized the laminar structure. The membrane with the highest performance among the as-prepared membranes exhibited a high water permeance of 90.5 L/m-2(-|-)h-1 bar-1 (which is twice that of the pristine Ti3C2Tx membrane) and good separation efficiency (methyl blue rejection rate: ∼99.8 %; Na2SO4 rejection rate: ∼5.0 %). Furthermore, the Fe3+-TA complex enhanced the membrane hydrophilicity, resulting in excellent antifouling properties. This study provides an environmentally friendly and facile method for fabricating two-dimensional loose nanofiltration membranes for textile wastewater treatment.

Fabrication of Loose Nanofiltration Membranes with High Rejection Selectivity between Natural Organic Matter and Salts for Drinking Water Treatment.

Loose nanofiltration (LNF) membranes with a molecular weight cut-off (MWCO) of about 1000 Da and high surface negative charge density have great application potential for drinking water treatment pursuing high rejection selectivity between natural organic matter (NOM) and mineral salts. This study was conducted to exploit the novel method coupling non-solvent induced phase separation (NIPS) and interfacial polymerization (IP) for the preparation of high-performance LNF membranes. A number of LNF membranes were synthesized by varying the polyethersulfone (PES) and piperazine (PIP) concentrations in the cast solution for the PES support layer preparation. Results showed that these two conditions could greatly affect the membrane water permeance, MWCO and surface charge. One LNF membrane, with a water permeance as high as 23.0 ± 1.8 L/m2/h/bar, when used for the filtration of conventional process-treated natural water, demonstrated a rejection of NOM higher than 70% and a low rejection of mineral salts at about 20%. Both the mineral salts/NOM selectivity and permselectivity were superior to the currently available LNF membranes as far as the authors know. This study demonstrated the great advantage of the NIPS-IP method for the fabrication of LNF membranes, particularly for the advanced treatment of drinking water.

Construction of Loose Positively Charged NF Membrane by Layer-by-Layer Grafting of Polyphenol and Polyethyleneimine on the PES/Fe Substrate for Dye/Salt Separation.

The effective separation of dyes and inorganic salts is highly desirable for recycling inorganic salts and water resource in printing and dyeing wastewater treatment. In this work, tannic acid (TA) and polyethyleneimine (PEI) were grafted on the PES/Fe ultrafiltration membrane via the coordination assembly and Michael addition strategy to fabricated a loose nanofiltration membrane (LNM). The effect of PEI concentration on membrane morphologies and properties was systematically investigated. The membrane surface becomes more hydrophilic and transforms into positive charge after the PEI grafting. The optimized PES/Fe-TA-PEI membrane possesses high pure water flux (124.6 L·m-2·h-1) and excellent dye rejections (98.5%, 99.8%, 98.4%, and 86.4% for Congo red, Eriochrome black T, Alcian blue 8GX, and Bromophenol blue, respectively) under 2 bar operation pressure. Meanwhile, the LNM showed a high Alcian blue 8GX rejection (>98.4%) and low NaCl rejection (<5.3%) for the dye/salt mixed solutions separation. Moreover, the PES/Fe-TA-PEI LNM exhibited good antifouling performance and long-term performance stability. These results reveal that such LNM shows great potential for effective fractionation of dyes and salts and recycling of textile wastewater.

Integrated loose nanofiltration-electrodialysis process for sustainable resource extraction from high-salinity textile wastewater.

Effective extraction of useful resources from high-salinity textile wastewater is a critical pathway for sustainable wastewater management. In this study, an integrated loose nanofiltration-electrodialysis process was explored for simultaneous recovery of dyes, NaCl and pure water from high-salinity textile wastewater, thus closing the material loop and minimizing waste emission. Specifically, a loose nanofiltration membrane (molecular weight cutoff of ~800 Da) was proposed to fractionate the dye and NaCl in the high-salinity textile wastewater. Through a nanofiltration-diafiltration unit, including a pre-concentration stage and a constant-volume diafiltration stage, the dye could be recovered from the high-salinity textile wastewater, being enriched at a factor of ~9.0, i.e., from 2.01 to 17.9 g·L-1 with 98.4% purity. Assisted with the subsequent implementation of electrodialysis, the NaCl concentrate and pure water were effectively reclaimed from the salt-containing permeate coming from the loose nanofiltration-diafiltration. Simultaneously, the produced pure water was further recycled to the nanofiltration-diafiltration unit. This study shows the potential of the integration of loose nanofiltation-diafiltration with electrodialysis for sufficient resource extraction from high-salinity textile wastewater.

Custom-Tailoring Loose Nanofiltration Membrane for Precise Biomolecule Fractionation: New Insight into Post-Treatment Mechanisms.

Loose nanofiltration (NF) membranes with diverse selectivity can meet the great demands in various bioseparation applications. Thus, a facile strategy to tune the properties such as pore size, surface charge, and hydrophilicity of the NF membrane is required to produce tailor-made loose NF membranes without changing the existing production line. Herein, we systematically investigated the post-treatment of the nascent poly(piperazine amide) NF membranes using different reagents (organic acids, weak bases, organic solvents and ionic liquid (IL)). Various characterizations revealed that the skin/separation layer became looser and permeance was promoted with the decrease of salt rejection in varying degrees. It was found that the O/N ratio did not rigorously represent the cross-linking degree of the skin layer, because besides the hydrolysis of the residual acyl chloride impeding the amido bond formation, the breaking of existing amido bonds and the grafting of free trimesoyl chloride molecules on the nascent membranes could also increase the O/N ratio during post-treatments. Then three mechanisms including hydrolysis, swelling rearrangement and capping reaction effects were proposed to better understand the membrane properties variations. All these effects resulted in larger pore size of the NF membrane, and the hydrolysis/capping effect might increase negative charge and hydrophilicity on the membrane, while the swelling rearrangement could produce less defective skin structure. These three effects might be involved together during a single treatment. Finally, the NF membrane post-treated by N-hexane could efficiently separate antibiotics and NaCl with the highest permeate flux, whereas the one post-treated by ionic liquid outperformed others for the decoloration of cane molasses (much more efficient than NF270, DL, and NTR7450 membranes). The long-term operating stability of the post-treated membranes selected was also confirmed by a continuous crossflow filtration for 15 h with regular alkaline cleaning.

Improvement of PVDF nanofiltration membrane potential, separation and anti-fouling performance by electret treatment.

Electret treatment was a simple method to enhance the charge-electrode properties of polyvinylidene fluoride (PVDF) materials due to the increase of space charge and polarization charge of PVDF materials. The polarization charge was due to the electric dipole orientation change in loose nanofiltration PVDF membrane, which increased the electric dipole moment and improved the polarity of surface potential. Importantly, electret charges were less affected by ambient humidity. Therefore, the electret treatment could improve the surface negative potential of loose nanofiltration PVDF membrane, so as to improve its anti-fouling performance under certain conditions. Based on the above theoretical analysis, the influence and mechanism of the electret treatment on the surface potential, morphology, structure, hydrophilicity and anti-pollution performance of PVDF membrane were studied in this manuscript. When the electret time was 7.5 min and the electret voltage was 30 kV, the surface negative potential was the highest. The content of ß phase crystals was 39.1%, which was 12.18% higher than that of untreated membrane. In addition, the surface morphology of PVDF membrane did not change significantly, but the water contact angle decreased slightly, and the pore size increased by 0.36-0.75 nm. Importantly, the flux and the rejection of dye and BSA increased to some extent, and the maximum rejection rate and water flux were increased by 10.34% and 20.25%, respectively. Through the cyclic filtration test and analysis, the anti-fouling performance of membrane was increased due to electrostatic repulsion.

High-Performance Polyacrylic Acid-Grafted PVDF Nanofiltration Membrane with Good Antifouling Property for the Textile Industry.

In the textile industry, a high-efficiency dye removal and low-retention of salt is demanded for recycling wastewater. In this study, polyvinylidene fluoride (PVDF) ultrafiltration membrane was transformed to a negatively charged loose nanofiltration (NF) membrane through UV-grafting of acrylic acid. At the optimal exposure of PVDF membrane in UV light for 5 min, the membrane had a high dye recovery above 99% (Congo red and Eriochrome® Black T) and a low sodium chloride (NaCl) rejection of less than 15% along with pure water flux of 26 L∙m-2∙h-1∙bar-1. Its antifouling and oleophobicity surface properties were verified using fluorescent- bovine serum albumin (BSA) and underwater mineral oil contact angle, respectively. According to the fluorescent microscopic images, the modified membrane had ten times lower adhesion of protein on the surface than the unmodified membrane. The underwater oil contact angle was raised from 110° to 155°. Moreover, the salt rejection followed this sequence: Na2SO4 > MgSO4 > NaCl > MgCl2, which agreed with the typical negatively charged NF membrane. In addition, the physicochemical characterization of membranes was further investigated to understand and link to the membrane performance, such as surface functional group, surface elements analysis, surface roughness/morphology, and surface hydrophilicity.

Bio-inspired co-deposited preparation of GO composite loose nanofiltration membrane for dye contaminated wastewater sustainable treatment.

The fully separation of dye/salt through loose nanofiltration membranes is of great significance for the sustainable development paradigm of textile wastewater. However, the current loose nanofiltration membranes suffer low separation efficiency and complex preparation. Herein, by one-step co-deposition, we develop graphene oxide (GO) composite loose nanofiltration membranes with low negatively charged surface. Our membrane possesses unconventional high pure water permeation of 71.7 LMH/bar, 92.9 % rejection for Methyl blue (MB) and 98.8 % rejection for Congo red (CR). Benefiting from the large interlayer distance of GO nanosheets and low negatively charged surface, membrane achieves high dyes/salts separation with satisfactory permeation to salts (94.3 % of Na2SO4, 97.6 % of MgSO4, 98.3 % of MgCl2 and 99.0 % of NaCl). The CR/salt mixed solutions exhibit similar removal rates to their constituents' single dye or salt solutions (CR rejection is up to more than 97 % and the permeations of all salts are above 93 %). At the same time, binary dyes mixtures (Congo red and Methyl orange) can also be effectively separated. Furthermore, the membrane shows a relatively desirable antifouling property. The flux recovery still remains at 85.9 % after three cycling filtrations. This study provides a facile approach to prepare highly-efficient loose nanofiltration membranes for wastewater sustainable remediation.

PIP/TMC Interfacial Polymerization with Electrospray: Novel Loose Nanofiltration Membrane for Dye Wastewater Treatment.

A loose nanofiltration (NF) membrane with excellent dye rejection and high permeation of inorganic salt is required to fractionate dye/salt mixture in dye wastewater treatment. In this study, we fabricated the loose NF membrane by using the electrospray interfacial polymerization (EIP) method. It is a novel and facile interfacial polymerization method, which controls the thickness of the poly(piperazine-amide) (PPA) layer in nanometers (1 nm/min) and changes cross-linking degree of PPA layer and pore size by varying the electrospray time; consequently, water permeance and dye/salt rejection ratio can be handled. The fabricated EIP membrane with an optimized fabrication condition (M30, electrospray time was 30 min) possessed excellent pure water permeance (20.2 LMH/bar), high dye rejection (e.g., 99.6% for congo red (CR)), and low salt rejection (e.g., 6.3% for NaCl). Moreover, the EIP membrane exhibited enhanced antifouling property than commercial NF membrane (NF90) with a high flux recovery rate (FRR) of 87.1% and low irreversible fouling (Rir) of 12.9% after fouled by bovine serum albumin (BSA) due to its great smooth surface (average roughness (Ra) is 12.2 nm), hydrophilicity property, enhanced zeta potential, and low protein adsorption. The results indicate that the EIP loose NF membrane had a high potential for dye wastewater treatment.