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Recent advances in nanotechnology have brought great opportunities to the developing next-generation nanofiltration membranes for addressing the concern of global water scarcity and energy crisis. Carbon dots have been deemed as a promising nanomaterial for enhancing the nanofiltration performance of polymeric membranes. Herein, carbon dots with cationic amine groups (PEI-CDs) and those with anionic sulfonate groups (PS-CDs) are incorporated into the polyamide selective layer of thin-film nanocomposite (TFN) membranes to create charged nanovoids (free volume) between the carbon dots and the surrounding polyamide network for high-efficiency nanofiltration. The positively charged amine group-based and negatively charged sulfonate group-based nanovoids in the resultant TFN-PEI-CDs and TFN-PS-CDs membranes, respectively, provide alternative pathways for efficient water permeation while effectively rejecting divalent ions via the Donnan and dielectric exclusion effects, thereby overcoming the recurring trade-off between permeability and selectivity encountered by dense polymeric membranes. In particular, the creation of negatively charged nanovoids enables the TFN-PS-CDs membrane to achieve one of the best performances among the recently reported nanofiltration membranes, by showing a nearly tripled pure water permeability of 30.9 L m−2 h−1 bar−1 as well as a higher Na 2 SO 4 rejection rate of 99.4% than the membrane with a pristine polyamide selective layer. Moreover, the TFN membranes demonstrate greater resistance to foulants with charges of the same sign as the nanovoids. This work provides insights into the design of nanovoids with desired properties in other polymeric membranes for high-efficiency filtration processes. [Display omitted] • Nanofiltration performance was improved by incorporating cationic and anionic CDs in the PA layer. • The ionic CDs created charged nanochannels between them and the surrounding PA matrix. • High pure water permeability of 30.9 L m−2 h−1 bar−1 and Na 2 SO 4 rejection rate of 99.4%. • Excellent filtration stability under different operating conditions and through a 14-day test. • Improved antifouling performance was demonstrated by using four types of ionic foulants. [ABSTRACT FROM AUTHOR]

Synthetic interlayers with multiple functions and structural stability have a high potential to construct novel thin film composite (TFC) membranes with demanding permselective property for precise separations. Herein, a functional interlayer derived from the polyelectrolyte-based layer-by-layer (LBL) self-assembly is reported to prepare interlayer engineered organic solvent nanofiltration (OSN) membranes using β-cyclodextrin (β-CD) as a monomer via interfacial polymerization (IP) process. Compared to the interlayer-free OSN membrane, a smoother selective layer with higher crosslinking degree is obtained for our developed membranes, enabling an improved organic dye rejection (e.g. , 91.9% for methyl orange and 98.8% for brilliant blue R). Importantly, the LBL-aided β-CD nanofilm exhibits competitive permeances towards both polar (e.g. , methanol, 5.8 LMH/bar) and nonpolar solvents (e.g. , hexane, 7.0 LMH/bar). These performances can be attributed to the multiple roles of LBL-based interlayer as preventing the intrusion of selective layer and creating dual linkages (i.e. , amide and ester), along with tailoring the physicochemical properties of caped β-CD nanofilm. Besides, the newly developed OSN membrane can discriminate between dye molecules with similar molecular weights and same charge but different molecular configurations. Meanwhile, its good structural integrity and long-term stability are also demonstrated by the 7-day filtration test using tetracycline in methanol and β-carotene in hexane, respectively, as evidence of constant solute rejections (≥90%) during the entire filtration process. This work unravels the functions of LBL-based interlayer in enhancing the OSN performance, offering new insights into shaping the development of interlayer engineered OSN membranes for real-life applications. [Display omitted] • An interlayer derived from polyelectrolyte-based LBL is constructed for OSN application. • The multiple roles of LBL-based interlayer in tailoring β-CD nanofilm are investigated. • Interlayered membranes possess high permeances for both polar and nonpolar solvents. • Structural integrity and long-term stability are confirmed by a 7-day filtration test. [ABSTRACT FROM AUTHOR]

The layer-by-layer (LbL) self-assembly is a common method for fabricating nanofiltration (NF) membranes. However, most multilayers are usually too thick and lack the necessary attributes to endow NF membranes with good permselectivity. In this study, we present a polyelectrolyte multilayered method by integrating dopamine as a "bio-glue". A three-step deposition was applied to the negatively charged PES substrate surface, following an alternate sequence of poly(allylamine hydrochloride) (PAH), dopamine (DA) and poly(sodium 4-styrenesulfonate) (PSS). The dopamine molecules were intercalated between the PAH and PSS layers to achieve a thinner thickness, higher hydrophilicity, smaller surface roughness and narrower pore size distribution. The resultant flat sheet (PAH/DA/PSS)4 polyelectrolyte multilayered (PEM) membranes exhibited enhanced water permeability (more than 60% increment from 13.5 to 21.9 LMH/bar) and higher rejection toward divalent ions (increasing MgCl 2 rejection from 91.0% to 94.8%) as compared with the control (PAH/PSS)4 NF membrane. Furthermore, the developed LbL method was applied on hollow fiber membrane modules and was able to achieve a higher Li+/Mg2+ selectivity from 15.6 to 37.8 and Na+/Mg2+selectivity from 11.0 to 19.1 using different simulated brines as feed solutions. On the whole, this polyelectrolyte multilayered method shows great potential for practical applications, including groundwater softening, seawater pretreatment and lithium extraction. [Display omitted] • A novel three-step LbL self-assembly method was proposed by integrating dopamine. • Dopamine intercalated selective layer exhibited a thinner and smoother surface. • The NF (PAH/DA/PSS)4 membrane showed better water permeability and higher divalent ion rejection. • Higher Na+/Mg2+ and Li+/Mg2+ selectivity was achieved due to the smaller pore size distribution. [ABSTRACT FROM AUTHOR]

Electrospun polymeric membranes are promising substrates for thin-film composite (TFC) membranes due to their unique interconnected pores and high porosity. However, it is still challenging to fabricate desirable electrospun substrates for organic solvent nanofiltration (OSN) owing to the relatively complex processing procedures and the organic operating environment. In this work, solvent-resistant electrospun polyimide (PI) nanofiber substrates were successfully fabricated through electrospinning followed by chemical cross-linking and heat-pressing. The cross-linking step improved the solvent tolerance of the membranes, while the heat-pressing step reduced the substrate pore size and surface roughness. However, it was found that heat-pressing at high temperatures (>140 °C) could degrade the cross-linking of PI, undermining their solvent-resistant property. A polyamide thin film layer was then synthesized on the solvent-resistant electrospun nanofibrous substrates via interfacial polymerization using reactant monomers m -phenylenediamine (MPD) and trimesoyl chloride (TMC). The TFC membranes exhibited excellent acetonitrile and acetone permeabilities of 31.28 ± 1.93 and 26.58 ± 1.13 L m−2 h−1 bar−1, respectively, with acid fuchsin (585 Da) and methyl orange (327 Da) rejections of 98.55 ± 1.24% and 92.42 ± 1.66%, respectively, in acetone. This study successfully demonstrated the potential use of electrospun PI nanofibers substrates for TFC membranes in OSN. [Display omitted] • Solvent resistant nanofibrous PI substrates were prepared by electrospinning followed by chemical cross-linking and heat-pressing. • Heat-pressing influenced the PI substrates' surface properties and solvent resistance, and the optimal point was 140 °C. • Polyamide thin film was synthesized on the PI substrates via interfacial polymerization for OSN application. • Acetone permeability was 26.58 L m−2 h−1 bar−1 with high rejection to acid fuchsin and methyl orange. [ABSTRACT FROM AUTHOR]