Hollow fiber nanofiltration membranes can withstand much higher foulant concentrations than their spiral wound counterparts and can be used in water purification without pretreatment. Still, the preparation of hollow fiber nanofiltration membranes is much less established. In this work, we demonstrate the design of a hollow fiber nanofiltration membrane with excellent rejection properties by alternatively coating a porous ultrafiltration membrane with a polycation, a polyzwitterion, and a polyanion. On model surfaces, we show, for the first time, that the polyzwitterion poly N-(3-sulfopropyl)-N-(methacryloxyethyl)-N,N-dimethylammonium betaine (PSBMA) can be incorporated into traditional polyelectrolyte multilayers based on poly(styrenesulfonate) (PSS) and poly(diallyldimethylammonium chloride) (PDADMAC). Furthermore, work on model surfaces allows a good characterization of, and insight into, the layer build-up and helps to establish the optimal membrane coating conditions. Membranes coated with these multilayers have high salt rejection of up to 42% NaCl, 72% CaCl2, and 98% Na2SO4 with permeabilities of 3.7-4.5 l·m(-2)·h(-1)·bar(-1). In addition to the salt rejections, the rejection of six distinctively different micropollutants, with molecular weights between 215 and 362 g·mol(-1), was investigated. Depending on the terminating layer, the incorporation of the polyzwitterion in the multilayer results in nanofiltration membranes that show excellent retentions for both positively and negatively charged micropollutants, a behavior that is attributed to dielectric exclusion of the solutes. Our approach of combining model surfaces with membrane performance measurements provides unique insights into the properties of polyzwitterion-containing multilayers and their applications.
We systematically investigate the assembly of multilayers based on a polyzwitterion (PSBMA) and a polycation (PDADMAC) for the development of ionic strength responsive membranes. Although the polyzwitterion is essentially charge neutral, we show that specific electrostatic interactions with the PDADMAC allow for the formation of stable multilayers. The growth of this LbL system is monitored on model surfaces (silica) via optical reflectometry for different pH values and ionic strengths. While no effect of pH on the layer growth is observed, we did observe a strong dependence on the ionic strength. Upon increasing the ionic strength during deposition from 0.005 to 0.5 M NaCl, the adsorbed amount is significantly decreased, a behavior that is opposite to classical LbL systems. Similar results to those obtained on silica are also observed on top of classical LbL systems and on polymeric membranes. This demonstrates that the growth of the polyzwitterion multilayers is independent of the substrate. Coating these polyzwitterion multilayers on hollow fiber membranes via dip-coating yields membranes that are stimuli responsive toward the ionic strength of the filtration solution, with an increase in permeability of up to 108% from 0 to 1.5 M NaCl. We show that the fabrication of the polyzwitterion multilayers is an easy and controlled way to provide surfaces, such as membranes, with the specific functionalities of polyzwitterions.
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