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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]

Abstract: The layer-by-layer (LBL) polyelectrolyte deposition was applied on polyethersulfone (PES) hollow fiber ultrafiltration membrane to prepare nanofiltration (NF) membrane for low pressure water softening application for the first time. The effects of polyelectrolyte type and molecular weight (MW), deposited bilayer number, polyelectrolyte solution pH and supporting electrolyte concentration on the performance of resultant membranes were studied thoroughly. Experiments revealed that the pH of the polyelectrolyte solution and supporting electrolyte concentration presented the most notable effects. For weak poly-cations, Poly(ethylenimine) (PEI) and Poly(allylamine hydrochloride) (PAH), the solution pH affected the membrane performance significantly, and high water permeability and divalent cation rejection were obtained at optimum pH values. Using a low concentration of supporting electrolyte at underneath layers was proved to be an effective way to increase water permeability while maintaining high salt rejection. A salt water flux (SWP) of 12LMH/bar and 94% Mg2+ rejection was obtained by depositing only two bilayers of PSS/PAH polyelectrolytes on the PES substrate, while for the 3000ppm mixed salt solution, the water permeability was 11LMH/bar with Mg2+ and Ca2+ rejection as high as 90%. These promising results demonstrate that LBL technique is potentially applicable for preparing low-pressure water softening hollow fiber membranes. [Copyright &y& Elsevier]