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Forward osmosis (FO) has been identified as an emerging technology for the concentration and crystallization of aqueous solutions at low temperatures. However, the application of the FO process has been limited due to the unavailability of a suitable draw solute. An ideal draw solute should be able to generate high osmotic pressure and must be easily regenerated with less reverse solute flux (RSF). Recently, hydrogels have attracted attention as a draw solution due to their high capacity to absorb water and low RSF. This study explores a poly (vinyl alcohol)/poly (diallyldimethylammonium chloride) (PVA-polyDADMAC) polymeric network hydrogel as a draw solute in forward osmosis. A low-pressure reverse osmosis (RO) membrane was used in the FO process to study the performance of the hydrogel prepared in this study as a draw solution. The robust and straightforward gel synthesis method provides an extensive-scale application. The results indicate that incorporating cationic polyelectrolyte poly (diallyldimethylammonium chloride) into the polymeric network increases swelling capacity and osmotic pressure, thereby resulting in an average water flux of the PVA-polyDADMAC hydrogel (0.97 L m[sup.−2] h[sup.−1]) that was 7.47 times higher than the PVA hydrogel during a 6 h FO process against a 5000 mg L[sup.−1] NaCl solution (as a feed solution). The effect of polymer and cross-linker composition on swelling capacity was studied to optimize the synthesized hydrogel composition. At 50 °C, the hydrogel releases nearly >70% of the water absorbed during the FO process at room temperatures, and water flux can be recovered by up to 86.6% of the initial flux after 12 hydrogel (draw solute) regenerations. Furthermore, this study suggests that incorporating cationic polyelectrolytes into the polymeric network enhances FO performances and lowers the actual energy requirements for (draw solute) regeneration. This study represents a significant step toward the commercial implementation of a hydrogel-driven FO system for the concentration of liquid-food extract.

Coacervation is a self-assembly strategy based on the complexation of polyelectrolytes, which is utilized in biomedicine and agriculture, as well as automotive and textile industries. In this paper, we developed a new approach to the on-demand periodic formation of polyelectrolyte complexes through a Liesegang-type hierarchical organization. Adjustment of reaction conditions allows us to assemble materials with a tunable spatiotemporal geometry and establish materials’ production cycles with a regulated periodicity. The proposed methodology allows the membrane to self-assemble when striving to reach balance and self-heal after exposure to external stimuli, such as potential difference and high pH. Using chronopotentiometry, K[sup.+] ion permeability behavior of the PEI–PSS coacervate membranes was demonstrated. The periodically self-assembled polyelectrolyte nanomembranes could further be integrated into novel energy storage devices and intelligent biocompatible membranes for bionics, soft nanorobotics, biosensing, and biocomputing.

There is notable discrepancy between experiments and coarse-grained model studies regarding the thermodynamic driving force in polyelectrolyte complex coacervation: experiments find the free energy change to be dominated by entropy, while simulations using coarse-grained models with implicit solvent usually report a large, even dominant energetic contribution in systems with weak to intermediate electrostatic strength. Here, using coarse-grained, implicit-solvent molecular dynamics simulation combined with thermodynamic analysis, we study the potential of mean force (PMF) in the two key stages on the coacervation pathway for symmetric polyelectrolyte mixtures: polycation–polyanion complexation and polyion pair–pair condensation.We show that the temperature dependence in the dielectric constant of water gives rise to a substantial entropic contribution in the electrostatic interaction. By accounting for this electrostatic entropy, which is due to solvent reorganization, we find that under common conditions (monovalent ions, room temperature) for aqueous systems, both stages are strongly entropy-driven with negligible or even unfavorable energetic contributions, consistent with experimental results. Furthermore, for weak to intermediate electrostatic strengths, this electrostatic entropy, rather than the counterion-release entropy, is the primary entropy contribution. From the calculated PMF, we find that the supernatant phase consists predominantly of polyion pairs with vanishingly small concentration of bare polyelectrolytes, and we provide an estimate of the spinodal of the supernatant phase. Finally, we showthat prior to contact, two neutral polyion pairsweakly attract each other by mutually induced polarization, providing the initial driving force for the fusion of the pairs.