Membranes are an attractive alternative to current thermal separations due to their scalability and energy efficiency in desalinating water. Unfortunately, many of the conventional membrane materials available today are unable to differentiate between ionic solutes, especially alkali cations, compromising their use in ion−ion separations. Inspired by the ion-specific interactions exhibited by biological ion channels, recent research efforts have focused on synthesizing and characterizing new polymeric materials that incorporate ligands into polymer networks to bias solubility and/or diffusivity of one cationic species over another. Despite these efforts, little is known about the influence of incorporating ligands into polymer membranes on solubility and diffusivity of the complexing species. In this study, we first build a qualitative model of salt partitioning, diffusivity, and permeability in generic cationcomplexing ligand-functionalized polymer membranes. Next, to validate our model and hypotheses, we perform atomistic molecular dynamics simulations of a 12-crown-4-functionalized membrane in the presence of alkali halide salts at low concentration. Generally, cation complexation enhances cation solubility but decreases diffusivity. Interestingly, the reduction in diffusivity is predicted to be larger than the enhancement in solubility for materials which operate by the mechanisms proposed in our physical picture, ultimately resulting in a reduction in the permeability of the selectively complexing ion.
Water swollen polymer networks are attractive for applications ranging from tissue regeneration to water purification. For water purification, charged polymers provide excellent ion separation properties. However, many ion exchange membranes (IEMs) are brittle, necessitating the use of thick support materials that ultimately decrease throughput. To this end, novel double network hydrogels (DNHs) with variable water content are prepared and characterized in terms of mechanical and ion transport properties to evaluate their potential utility as tough membrane materials. The first network contains fixed anionic charges, while the other is comprised of a copolymer with varied ratios of hydrophobic ethyl acrylate (EA) and hydrophilic dimethyl acrylamide (DMA) repeat units. Characterization of freestanding DNH films reveals a reduction in water content from 88 to 53 wt% and a simultaneous increase in ultimate stress and strain by ~3.5× and ~4.5×, respectively, for 95%/5% EA/DMA, relative to 100% DMA. Fundamental salt transport properties relevant to water purification, including permeability, solubility, and diffusivity, are measured and systematically compared with conventional membrane materials to inform the development of DNHs for membrane applications. The ability to simultaneously reduce water content and increase mechanical integrity highlights the potential of DNHs as a synthetic platform for future membrane applications.
Water swollen polymer networks are attractive for applications ranging from tissue regeneration to water purification. For water purification, charged polymers provide excellent ion separation properties. However, many ion exchange membranes (IEMs) are brittle, necessitating the use of thick support materials that ultimately decrease throughput. To this end, a series of double network hydrogels (DNHs), synthesized with varied composition to decrease water content, are examined as robust membrane materials for water purification. One network contains fixed anionic charges, while the other comprises a copolymer with different ratios of hydrophobic ethyl acrylate (EA) and hydrophilic dimethyl acrylamide (DMA) repeat units. Characterizing water content and mechanical performance in free standing DNH films reveals a ~5× decrease in water content, while increasing ultimate stress and strain by ~3.5× and ~4.5× for 90:5 EA:DMA relative to pure DMA. Salt transport properties relevant to water purification, including permeability, solubility, and diffusivity, are measured and show improved performance upon reducing water content. Overall, the ability to simultaneously reduce water content, increase mechanical integrity, and decrease salt transport rates highlights the potential of DNHs for membrane applications.
Water swollen polymer networks are attractive for applications ranging from tissue regeneration to water purification. For water purification, charged polymers provide excellent ion separation properties. However, many ion exchange membranes (IEMs) are brittle, necessitating the use of thick support materials that ultimately decrease throughput. To this end, a series of double network hydrogels (DNHs), synthesized with varied composition to decrease water content, are examined as robust membrane materials for water purification. One network contains fixed anionic charges, while the other comprises a copolymer with different ratios of hydrophobic ethyl acrylate (EA) and hydrophilic dimethyl acrylamide (DMA) repeat units. Characterizing water content and mechanical performance in free standing DNH films reveals a ~5× decrease in water content, while increasing ultimate stress and strain by ~3.5× and ~4.5× for 90:5 EA:DMA relative to pure DMA. Salt transport properties relevant to water purification, including permeability, solubility, and diffusivity, are measured and show improved performance upon reducing water content. Overall, the ability to simultaneously reduce water content, increase mechanical integrity, and decrease salt transport rates highlights the potential of DNHs for membrane applications.
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