Polyphenol-mediated defect patching of graphene oxide membranes for sulfonamide contaminants removal and fouling control.

Graphene oxide (GO)-based laminar membranes are promising candidates for next-generation nanofiltration membranes because of their theoretically frictionless nanochannels. However, nonuniform stacking during the filtration process and the inherent swelling of GO nanosheets generate horizontal and vertical defects, leading to a low selectivity and susceptibility to pore blockage. Herein, both types of defects are simultaneously patching by utilizing tannic acid and FeⅢ. Tannic acid first partially reduced the upper GO framework, and then coordinated with FeⅢ to form a metal-polyphenol network covering horizontal defects. Due to the enhanced steric hindrance, the resulting membrane exhibited a two-fold increase in sulfonamide contaminants exclusion compared to the pristine GO membrane. A non-significant reduction in permeance was observed. In terms of fouling control, shielding defects significantly alleviated the irreversible pore blockage of the membrane. Additionally, the hydrophilic metal-polyphenol network weakened the adhesion force between the membrane and foulants, thereby improving the reversibility of fouling in the cleaning stage. This work opens up a new way to develop GO-based membranes with enhanced separation performance and antifouling ability.

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.

Positively charged membranes for dye/salt separation based on a crossover combination of Mannich reaction and prebiotic chemistry.

With the advent of increasingly loose nanofiltration membranes for dye desalination, synthesis methods based on interfacial polymerization and bio-inspired materials such as polydopamine (pDA) have been investigated. However, the long polymerization time of pDA greatly limits the synthesis and application of fast dye/salt separation membranes. In this work, prebiotic chemistry-inspired aminomalononitrile (AMN) was used as a binder to co-deposit the Mannich reaction of tetrakis(hydroxymethyl)phosphonium chloride (THPC) and polyethyleneimine (PEI) to form the positively charged selective layer rapidly. The optimum membrane had a water permeance of 30.7 LMH bar-1 and a rejection of positively charged Victoria blue B (VBB, 200 ppm) and Na2SO4 (1 g/L) of 99.5 % and 9.9 %, respectively. Moreover, the results of a practical application test showed that it had excellent separation performance towards various positively charged dyes and salts. In addition, the actual application test results show that the membrane has good long-term stability during application. In terms of antifouling and antibacterial, the membrane has excellent antibacterial and antifouling properties., Further antibacterial tests were carried out, and the inactivation effect of the membrane on E. coli was also confirmed. The preparation method proposed in this work provides technical support for developing new dye/salt separation membranes.

A PEI/TMC membrane modified with an ionic liquid with enhanced permeability and antibacterial properties for the removal of heavy metal ions.

Heavy metal ions in drinking water severely threaten public health in various places worldwide. Nanofiltration (NF) membrane technology is an attractive option for heavy metal ions removal; however, improving NF membrane filtration performance is required to make their industrial application viable. In this study, a positively charged THPC/PEI-TMC NF membrane was designed via simple one-step incorporation of Tetrakis (hydroxymethyl) phosphonium chloride (THPC) biocide on the surface of PEI-TMC membranes, significantly optimizing surface morphology, roughness, hydrophilicity, and zeta potential of PEI-TMC membranes. It was found that the pure water permeability (11.6 Lm-2h-1bar-1) of the THPC modified membrane was three times larger than that of the original PEI-TMC membrane (3.4 Lm-2h-1bar-1) while maintaining a high level of ion rejections (around 95% for Zn2+, Cd2+, Ni2+, Cu2+ and about 90% for Pb2+). Additionally, the incorporation of the THPC on the original PEI-TMC membrane surface also conferred good antibacterial properties, which protect the organic membrane from bacterial growth and prolong the lifespan of the membrane.

A novel ceramic-based thin-film composite nanofiltration membrane with enhanced performance and regeneration potential.

The rational design of a ceramic-based nanofiltration membrane remains a significant challenge due to its performance and fabrication cost. Herein, we report a high-performance ceramic-based thin-film composite (TFC) membrane fabricated via a typical interfacial polymerization on an interwoven net substrate assembled by titanium dioxide (TiO2) nanowires. The chemical properties and morphologies were systematically investigated for ceramic substrates and their corresponding TFC membranes. Due to the significantly improved hydrophilicity of the TiO2 framework, more reactive amine monomers were uniformly adsorbed on the modified surface of the ceramic substrate, yielding an ultrathin polyamide layer with less resistance. In addition, the smooth surface and decreased pore size of the TiO2 framework contributed to forming a defect-free polyamide layer. As a result, the obtained ceramic-based TFC membrane evinced high permeance of 26.4 L m-2 h-1 bar-1 and excellent salt rejection efficiency, leading to simultaneous improvements compared with the control TFC membrane without the TiO2 framework. Notably, the potential regeneration ability of the ceramic-based TFC membrane could be achieved via facile low-temperature calcination and re-polymerization process due to the varied thermostability between the polyamide layer and the robust ceramic substrate. The operation of regeneration helped to prolong the lifetime and decrease the cost for the ceramic-based TFC membrane. This research provides a feasible protocol to fabricate sustainable ceramic-based nanofiltration membranes with enhanced performance for water treatment.

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.

Thin-Film Composite Membrane Prepared by Interfacial Polymerization on the Integrated ZIF-L Nanosheets Interface for Pervaporation Dehydration.

Thin-film composite (TFC) membranes are attracting wide attention because their ultrathin selective layer usually corresponds to the higher membrane flux for pervaporation. However, the direct preparation of the TFC membranes on ceramic substrates confronted with the great difficulties because the larger pores on ceramic substrate surfaces are detrimental to the formation of an intact polyamide (PA) selective layer produced by interfacial polymerization (IP) reaction. Here, the integrated ZIF-L nanosheets were proposed to be used as an assistance interlayer for the first time to eliminate the existence of the pores of the ceramic support, and provides a better basis for the formation of an intact PA selective layer by IP reaction between TMC and ethylenediamine (EDA). The experimental data obtained in pervaporation (PV) show that the increased flux from 1.1 to 2.9 kg/m2h corresponds to the decreased separation factor from 396 to 110 when the feed concentration of ethanol decreases from 95 wt % to 80 wt % at 50 °C. In addition, the membrane flux increases from 0.8 to 2.5 kg/m2h with a change of the separation factor from 683 to 111 when the operational temperature varies from 30 to 60 °C. These results demonstrate the great potential of the fabricated TFC membranes in practical application for PV dehydration of organic solutions.

Tailoring Charged Nanofiltration Membrane Based on Non-Aromatic Tris(3-aminopropyl)amine for Effective Water Softening.

High-performance positively-charged nanofiltration (NF) membranes have a profound significance for water softening. In this work, a novel monomer, tris(3-aminopropyl)amine (TAEA), with one tertiary amine group and three primary amine groups, was blended with trace amounts of piperazine (PIP) in aqueous solution to fabricate a positively-charged NF membrane with tunable performance. As the molecular structures of TAEA and PIP are totally different, the chemical composition and structure of the polyamine selective layer could be tailored via varying the PIP content. The resulting optimal membrane exhibited an excellent water permeability of 10.2 LMH bar-1 and a high rejection of MgCl2 (92.4%), due to the incorporation of TAEA/PIP. In addition, this TAEA NF membrane has a superior long-term stability. Thus, this work provides a facile way to prepare a positively charged membrane with an efficient water softening ability.

Surface modification of poly(vinylidene fluoride) hollow fibre membranes for biogas purification in a gas-liquid membrane contactor system.

The wetting of hollow fibre membranes decreases the performance of the liquid-gas membrane contactor for CO2 capture in biogas upgrading. To solve this problem, in this work, a poly(vinylidene fluoride) (PVDF) hollow fibre membrane for a liquid-gas membrane contactor was coated with a superhydrophobic layer composed of a combination of hydrophobic SiO2 nanoparticles and polydimethylsiloxane (PDMS) by the method of spray deposition. A rough layer of SiO2 deposited on the PVDF membrane resulted in an enhanced surface hydrophobicity. The surface structure of the pristine PVDF significantly affected the homogeneity of the generated SiO2 layer. A uniform surface coating on the PVDF upper layer resulted from the presence of micrometre and nanometre-sized roughness on the surface of the PVDF membrane, which was achieved with a SiO2 concentration of 4.44 mg ml-1 (0.2 g/45 ml) in the coating solution. As a result, the water contact angle of the modified surface was recorded as 155 ± 3°, which is higher than that of the pristine surface. The high contact angle is advantageous for reducing the wetting of the membrane. Additional mass transfer resistance was introduced by the superhydrophobic layer. In addition, continuous CO2 absorption tests were carried out in original and modified PVDF hollow fibre membrane contactors, using monoethanolamine (MEA) solution as the absorbent. A long-term stability test revealed that the modified PVDF hollow fibre membrane contactor was able to outperform the original membrane contactor and demonstrated outstanding long-term stability, suggesting that spray deposition is a promising approach to obtain superhydrophobic PVDF membranes for liquid-gas membrane absorption.