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Tuning the charge of polyelectrolyte complex membranes prepared via aqueous phase separation.

ABSTRACT: In this work, polyelectrolyte mixing ratio is studied as a tuning parameter to control the charge, and thus the separation properties of polyelectrolyte complex (PEC) membranes prepared via Aqueous Phase Separation (APS). In this approach, various ratios of poly(sodium 4-styrenesulfonate) (PSS) and poly(diallyldimethylammonium chloride) (PDADMAC) are mixed at high salinity and the PEC-based membranes are then precipitated using low salinity coagulation baths. The monomeric ratio of PSS to PDADMAC is varied from 1.0 : 0.8 through to 1.0 : 1.2. Obtained membranes have an asymmetric structure and function as nanofiltration membranes with on average 1 L m^-2 h^-1 bar^-1 pure water permeance and <400 Da molecular weight cut-off (MWCO); except for the 1.0 : 1.2 membrane, where the water permeance was much higher (>20 L m^-2 h^-1 bar^-1) with a similarly low MWCO. For the first time, we report the formation of both negatively and positively charged PSS-PDADMAC based APS membranes, as determined by both streaming potential and salt retention measurements. We hypothesize that the salt type used in the APS process plays a key role in the observed change in membrane charge. The point where the membrane charge transitions from negative to positive is found to be between the 1.0 : 0.9 and 1.0 : 1.0 PSS : PDADMAC ratios. The polyelectrolyte ratio not only affects membrane charge, but also their mechanical properties. The 1.0 : 0.9 and 1.0 : 1.0 membranes perform the best amongst the membranes prepared in this study since they have high salt retentions (up to 90% Na₂SO₄ and 75% MgCl₂, respectively) and better mechanical stability. The higher permeance of the more charged, and thus more swollen, 1.0 : 0.8 and 1.0 : 1.2 membranes provide a relevant new direction for the development of APS-based PEC membranes.

SUBMITTER: Durmaz EN

PROVIDER: S-EPMC8549507 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:In the single-polyelectrolyte aqueous phase separation (APS) approach, membranes are prepared by precipitating a weak polyelectrolyte from a concentrated aqueous solution using a pH switch. This has proven to be a versatile and more sustainable method compared to conventional approaches as it significantly reduces the use of organic solvents. Poly(styrene-alt-maleic acid) (PSaMA) is a polymer that has been extensively investigated for APS and has been the basis for both open and dense membranes with good performances. These membranes are chemically crosslinked and, in this work, we further investigated ultrafiltration (UF) and nanofiltration (NF) membranes prepared with PSaMA for their stability in various organic solvents and under different pH conditions. It was shown that these membranes had stable performances in both isopropanol (IPA) and toluene, and a slightly reduced performance in N-methyl-2-pyrollidone (NMP). However, PSaMA did not perform well as a selective layer in these solvents, indicating that the real opportunity would be to use the UF-type PSaMA membranes as solvent-stable support membranes. Additionally, the membranes proved to be stable in an acidic-to-neutral pH regime (pH 2-7); and, due to the pH-responsive nature of PSaMA, for the NF membranes, a pH-dependent retention of Mg2+ and SO42- ions was observed and, for the UF membranes, a strong responsive behavior was observed, where the pH can be used to control the membrane permeability. However, long-term exposure to elevated pH conditions (pH 8-10) resulted in severe swelling of the NF membranes, resulting in defect formation, and compaction of the UF membranes. For the UF membranes, this compaction did prove to be reversible for some but not all of the membrane samples measured. These results showed that in aqueous systems, membranes prepared with PSaMA had interesting responsive behaviors but performed best at neutral and acidic pH values. Moreover, the membranes exhibited excellent stability in the organic solvents IPA and toluene.

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Tuning the charge of polyelectrolyte complex membranes prepared via aqueous phase separation.

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