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[Display omitted] • Nanofiltration (NF) membranes were prepared using hydroxypropyltrimethyl ammonium chloride chitosan (HACC) as aqueous phase co-monomer. • The surface electropositivity of NF membrane was significantly enhanced with almost constant pore size. • Modified NF membranes demonstrated superb magnesium-lithium separation performance and excellent antibacterial properties. In recent years, the global demand for lithium resources has been constantly rising thanks to the rapid development of the new energy industry. Nanofiltration (NF) membranes with positive charge could achieve high efficiency separation performance of magnesium ion (Mg2+)/ lithium ion (Li+), which provides a useful solution for the extraction and recovery of lithium resources from brine. In this work, hydroxypropyltrimethyl ammonium chloride chitosan (HACC) was introduced into the interfacial polymerization (IP) as co-monomer with piperazine (PIP) to react with trimesoyl chloride (TMC) for preparing positively charged NF membranes. Based on the modulation of IP process by HACC, the thickness of the modified NF membrane separation layer reduced and the hydrophilicity increased, while the pore size had no obvious variation. In addition, the introduction of the quaternary ammonium group in HACC also increased the antibacterial properties of the NF membrane. The optimized NF-HACC-0.3 not only improved the separation factor significantly, but also increased the flux by 2 times compared with the original membrane. This strategy provides a new valuable idea and insight for the preparation and development of Mg2+/Li+ separation NF membranes. [ABSTRACT FROM AUTHOR]

The regulation of interfacial polymerization (IP) is the critical procedure for the preparation and industrialization of thin film composite (TFC) nanofiltration (NF) membranes. However, the IP control is still a huge challenge based on the extremely rapid reaction rate during the fabrication of the membrane. Herein, a new strategy was developed to modulate the IP process to increase the NF membrane performance. The aldehyde oxidized dextran (ODex) interlayer was deposited on the polysulfone ultrafiltration substrate, and the enamine would form between the secondary amines of aqueous phase monomer piperazine (PIP) and aldehyde groups of the ODex. Based on the by-products of IP, the enamine gradually decomposed reversibly in a hydrogen ion environment and the immobilized PIP was released and continued to react with organic phase monomer trimesoyl chloride (TMC). Accordingly, a thinner and exhibiting nanowire structures separation layer with fewer defects was obtained. The permeance of the optimal NF membrane with 0.7 wt% ODex interlayer deposition concentration could reach up to 208 ± 10.4 Lm−2h−1MPa−1, which was more than 2.5 times permeance of the ordinary NF membrane, and the rejection rate for Na 2 SO 4 could reach 99.3 ± 0.3%. In addition, the mono- and divalent ion selectivity of the modified membrane was also greatly improved (α NaCl/Na2SO4 = 115). This study provides a new idea for the regulation of IP process, thereby suggesting a reasonable proposal for improving the performance of TFC NF membranes. [Display omitted] •The enamine was formed between the secondary amines of piperazine and the aldehyde group on the oxidized dextran interlayer. •The interfacial polymerization procedure was effectively regulated by a reversible enamine reaction. •The effect of enamine reversible reaction on the structure of nanofiltration membrane was discussed in detail. •The performance of modified NF membranes for monovalent/divalent salts selectivity was significantly improved. [ABSTRACT FROM AUTHOR]

[Display omitted] • Carboxylated starch nanoparticles (CSNPs) were synthesized and embedded in the separation layer of the nanofiltration membrane. • The aggregated or large CSNPs adsorb the aqueous phase to build an aqueous template during the interfacial polymerization transferring the reaction interface. • The compatibility problem of nanoparticles and separation layer was effectively solved. • The S NaCl/Na2SO4 of the modified nanofiltration membrane reached 180 with more than 2 times improvement in flux. The challenge of poor compatibility between nanoparticles and separation layers in thin film nanocomposite (TFN) nanofiltration (NF) membranes has always plagued the researchers. In this work, a carboxylated starch nanoparticles (CSNPs) were introduced into the polyamide (PA) separation layer of NF membrane by the IP reaction between trimesoyl chloride (TMC) and piperazine (PIP). The agglomerated or large size CSNPs could transfer the reaction interface above the particles through the formation of a water template by adsorption of aqueous phase monomers, which shaped the defect-free separation layer. Furthermore, the reduced thickness and increased density of the separation layer greatly enhanced the separation selectivity of the nanofiltration membrane thanks to the introduction of hydrophilic groups of nanoparticles. The modified membrane achieved a nearly 5-fold improvement in separation selectivity for NaCl and Na 2 SO 4 (S NaCl/Na2SO4 = 180) and a 2-fold increase in the water permeance. In addition, the modified NF membrane also possessed better chlorine-resistance property based on the formation of polyarylester between the reaction of hydroxyl groups in CSNPs and acyl chloride groups in TMC. Such novel aqueous-phase additives provide new insights to effectively solve the compatibility problem between the nanoparticles and separation layers, which is favorable for the commercial production of NF membrane. [ABSTRACT FROM AUTHOR]

The thin-film composite (TFC) nanofiltration (NF) membrane is a novel kind of membrane that has been extensively studied in recent years and broadly applied in desalination and wastewater treatment. The improvement of separation performance by optimizing the structure and morphology of NF membranes can significantly reduce energy consumption and bring more economic benefits. In this work, glutaraldehyde (GA) was used to crosslink polyethyleneimine (PEI) and dextran nanoparticles (DNPs) to construct an interfacial coating interlayer on polysulfone (PSF) ultrafiltration (UF) substrate. Subsequently, the polyamide (PA) NF membranes were fabricated by interfacial polymerization (IP) between piperazine (PIP) and trimesoyl chloride (TMC). DNPs were semi-encapsulated in the PEI coating and the exposed nanoparticles would be embedded in the PA layer for forming interfacial channels after IP. The interlayer not only affected the adsorption and diffusion of aqueous phase monomers to form a thin membrane, but also improved the membrane density to prevent selective defects associated with the incorporation of nanoparticles. The pure water permeance of the interlayered-TFC NF membrane was determined as 313.3 Lm−2h−1MPa−1, which was approximately four-fold that of the pristine membrane. The retention rate of various divalent salts of the NF membrane also significantly improved, and the retention rate of Na 2 SO 4 exceeded 99%. This innovative method of interlayer modification has exhibited great potential in rapid desalination and wastewater recovery, providing new possibilities for the preparation of industrial high-performance NF membranes. [Display omitted] • An innovative interlayer combining DNPs and PEI coating was successfully constructed. • DNPs were semi-encapsulated in the PEI coating to formed interfacial channels favorable for water passage. • The flux of the interlayer-modified NF membrane increased nearly 4 times with the retention rate of Na 2 SO 4 above 99%. • NF membrane exhibited excellent monovalent/divalent ion selectivity. [ABSTRACT FROM AUTHOR]

The thin-film composite (TFC) nanofiltration (NF) membrane is an excellent choice to solve water shortage based on the advantages of high flux and selective separation. However, the current NF membrane still causes a tremendous amount of energy consumption in the practical applications due to the limitation of flux. In this work, dextran nanoparticles (DNPs) with the cross-linked organic components, numerous hydrophilic groups and internal cavities were added into the aqueous phase solution, and novel NF membranes were fabricated by adjusting the concentration and particle size of DNPs to control the interfacial polymerization (IP) reaction. After modification, the decrease of membrane thickness and the increase of surface hydrophilicity improved the separation performance of NF membrane. The water flux of NF membrane with 0.5 wt% DNPs doping was up to 211.2 Lm−2h−1MPa−1, which was more than twice as high as the unmodified membrane with Na 2 SO 4 retention up to above 98%. It was also worth mentioning that the modified membrane indicated excellent monovalent/divalent ion selectivity and anti-fouling performance. This strategy of improving membrane performance by controlling the concentration and particle size of the aqueous phase additives with the advantages of simplicity and universality provides a certain impetus for the development of TFC membrane. • Dextran nanoparticles were successfully incorporated into the separation layer of NF membrane. • The water flux of the DNPs-modified NF membrane increased 2–3 times without sacrificing the Na 2 SO 4 retention. • The influence of the particle size and concentration of DNPs was discussed detailedly. • The anti-fouling performance and monovalent/divalent ion selectivity of the membrane improved. [ABSTRACT FROM AUTHOR]

Nanofiltration (NF) membrane is of great significance for desalination of light brine and purification of drinking water. Although the development of novel preparation methods and membrane materials has improved the separation performance, it is still a major challenge to promote NF membrane toward industrial production with simpler and more controllable process. Herein, the polyphenol intermediate layer was designed by 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethyl-1,1′-spirobisindane (TTSBI) with twist structure and polyethyleneimine (PEI) co-deposition to increase the surface hydrophilicity and electropositivity of the polysulfone ultrafiltration substrate. Subsequently interfacial polymerization (IP) was carried out on the polyphenol intermediate layer to assemble a polyamide ultrathin selective layer using trimesoyl chloride and piperazine monomer. Through adjusting the co-deposition time of TTSB and PEI, a unique nano-pleated structure was successfully formed on the thin-film composite membrane surface. The water permeance of the membrane was determined as 23.7 L m−2 h−1 bar−1 with 99.4% Na 2 SO 4 rejection, which was almost triple fold of the flux of the controller membrane without the intermediate layer. Our results provide an efficient and convenient way to fabricate the advanced NF membrane with higher divalent/monovalent ion selectivity and water permeance simultaneously, which will provide advices for the gas separation and pervaporation membranes with the IP method. • Novel TTSBI-PEI interlayer-based polyamide membrane was fabricated by interfacial polymerization. • The nano-pleated structure on the selective layer improved the water flux without deterioration of Na 2 SO 4 rejection. • The novel nanofiltration membrane exhibited excellent long-term stability. [ABSTRACT FROM AUTHOR]