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  1. Article ; Online: Enhancing the Separation Performance of Aqueous Phase Separation-Based Membranes through Polyelectrolyte Multilayer Coatings and Interfacial Polymerization.

    Baig, Muhammad Irshad / Willott, Joshua D / de Vos, Wiebe M

    ACS applied polymer materials

    2021  Volume 3, Issue 7, Page(s) 3560–3568

    Abstract: The aqueous phase separation (APS) technique allows membrane fabrication without use of unsustainable organic solvents, while at the same time, it provides extensive control over membrane pore size and morphology. Herein, we investigate if ... ...

    Abstract The aqueous phase separation (APS) technique allows membrane fabrication without use of unsustainable organic solvents, while at the same time, it provides extensive control over membrane pore size and morphology. Herein, we investigate if polyelectrolyte complexation-induced APS ultrafiltration membranes can be the basis for different types of nanofiltration membranes. We demonstrate that APS membranes can be used as support membranes for functional surface coatings like thin polyelectrolyte multilayer (PEMs) and interfacial polymerization (IP) coatings. Three different PEMs were fabricated on poly(sodium 4-styrene sulfonate) (PSS) poly(allylamine hydrochloride) (PAH) APS ultrafiltration membranes, and only 4.5 bilayers were needed to create nanofiltration membranes with molecular weight cut-off (MWCO) values of 210-390 Da while maintaining a roughly constant water permeability (∼1.7 L·m
    Language English
    Publishing date 2021-06-18
    Publishing country United States
    Document type Journal Article
    ISSN 2637-6105
    ISSN (online) 2637-6105
    DOI 10.1021/acsapm.1c00457
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Solvent and pH Stability of Poly(styrene-alt-maleic acid) (PSaMA) Membranes Prepared by Aqueous Phase Separation (APS).

    Nielen, Wouter M / Willott, Joshua D / de Vos, Wiebe M

    Membranes

    2021  Volume 11, Issue 11

    Abstract: 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 ... ...

    Abstract 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 Mg
    Language English
    Publishing date 2021-10-29
    Publishing country Switzerland
    Document type Journal Article
    ISSN 2077-0375
    ISSN 2077-0375
    DOI 10.3390/membranes11110835
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Polyelectrolyte Complex Hollow Fiber Membranes Prepared via Aqueous Phase Separation.

    Baig, Muhammad Irshad / Pejman, Mehdi / Willott, Joshua D / Tiraferri, Alberto / de Vos, Wiebe M

    ACS applied polymer materials

    2022  Volume 4, Issue 2, Page(s) 1010–1020

    Abstract: Hollow fiber (HF) membrane geometry is the preferred choice for most commercial membrane operations. Such fibers are conventionally prepared via the non-solvent-induced phase separation technique, which heavily relies on hazardous and reprotoxic organic ... ...

    Abstract Hollow fiber (HF) membrane geometry is the preferred choice for most commercial membrane operations. Such fibers are conventionally prepared via the non-solvent-induced phase separation technique, which heavily relies on hazardous and reprotoxic organic solvents such as
    Language English
    Publishing date 2022-01-11
    Publishing country United States
    Document type Journal Article
    ISSN 2637-6105
    ISSN (online) 2637-6105
    DOI 10.1021/acsapm.1c01464
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: Comparing polymer-surfactant complexes to polyelectrolytes.

    Gresham, Isaac J / Johnson, Edwin C / Robertson, Hayden / Willott, Joshua D / Webber, Grant B / Wanless, Erica J / Nelson, Andrew R J / Prescott, Stuart W

    Journal of colloid and interface science

    2023  Volume 655, Page(s) 262–272

    Abstract: Hypothesis: Understanding the complex interactions between polymers and surfactants is required to optimise commercially relevant systems such as paint, toothpaste and detergent. Neutral polymers complex with surfactants, forming 'pearl necklace' ... ...

    Abstract Hypothesis: Understanding the complex interactions between polymers and surfactants is required to optimise commercially relevant systems such as paint, toothpaste and detergent. Neutral polymers complex with surfactants, forming 'pearl necklace' structures that are often conceptualised as pseudo-polyelectrolytes. Here we pose two questions to test the limits of this analogy: Firstly, in the presence of salt, do these polymer-surfactant systems behave like polyelectrolytes? Secondly, do polymer-surfactant complexes resist geometric confinement like polyelectrolytes?
    Experiments: We test the limits of the pseudo-polyelectrolyte analogy through studying a poly(N-isopropylacrylamide) (PNIPAM) brush in the presence of sodium dodecylsulfate (SDS). Brushes are ideal for interrogating pseudo-polyelectrolytes, as neutral and polyelectrolyte brushes exhibit distinct and well understood behaviours. Spectroscopic ellipsometry, quartz crystal microbalance with dissipation monitoring (QCM-D), and neutron reflectometry (NR) were used to monitor the behaviour and structure of the PNIPAM-SDS system as a function of NaCl concentration. The ability of the PNIPAM-SDS complex to resist geometric confinement was probed with NR.
    Findings: At a fixed SDS concentration below the zero-salt CMC, increasing NaCl concentration <100 mM promoted brush swelling due to an increase in osmotic pressure, not dissimilar to a weak polyelectrolyte. At these salt concentrations, the swelling of the brush could be described by a single parameter: the effective CMC. However, at high NaCl concentrations (e.g., 500 mM) no brush collapse was observed at all (non-zero) concentrations of SDS studied, contrary to what is seen for many polyelectrolytes. Study of the polymer-surfactant system under confinement revealed that the physical volume of surfactant dominates the structure of the strongly confined system, which further differentiates it from the polyelectrolyte case.
    Language English
    Publishing date 2023-10-23
    Publishing country United States
    Document type Journal Article
    ZDB-ID 241597-5
    ISSN 1095-7103 ; 0021-9797
    ISSN (online) 1095-7103
    ISSN 0021-9797
    DOI 10.1016/j.jcis.2023.10.101
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Aqueous Phase Separation of Responsive Copolymers for Sustainable and Mechanically Stable Membranes.

    Nielen, Wouter M / Willott, Joshua D / de Vos, Wiebe M

    ACS applied polymer materials

    2020  Volume 2, Issue 4, Page(s) 1702–1710

    Abstract: Membranes are often used in environmentally friendly applications and as a sustainable alternative to conventional processes. Unfortunately, the vast majority of polymeric membranes are produced via an unsustainable and environmentally unfriendly process ...

    Abstract Membranes are often used in environmentally friendly applications and as a sustainable alternative to conventional processes. Unfortunately, the vast majority of polymeric membranes are produced via an unsustainable and environmentally unfriendly process that requires large amounts of harsh reprotoxic chemicals such as
    Language English
    Publishing date 2020-03-06
    Publishing country United States
    Document type Journal Article
    ISSN 2637-6105
    ISSN (online) 2637-6105
    DOI 10.1021/acsapm.0c00119
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Effect of Solution Viscosity on the Precipitation of PSaMA in Aqueous Phase Separation-Based Membrane Formation.

    Nielen, Wouter M / Willott, Joshua D / Galicia, Julia A R / de Vos, Wiebe M

    Polymers

    2021  Volume 13, Issue 11

    Abstract: Aqueous phase separation (APS) is a recently developed sustainable alternative to the conventional organic solvent based nonsolvent-induced phase separation (NIPS) method to prepare polymeric membranes. In APS, polyelectrolytes are precipitated from ... ...

    Abstract Aqueous phase separation (APS) is a recently developed sustainable alternative to the conventional organic solvent based nonsolvent-induced phase separation (NIPS) method to prepare polymeric membranes. In APS, polyelectrolytes are precipitated from aqueous solutions through pH or salinity switches. Although APS differs from NIPS in the polymer and solvents, they share many tuning parameters. In this work, we investigate the APS-based preparation of membranes from poly(styrene-alt-maleic acid) (PSaMA) with a focus on acid concentration in the coagulation bath, and polymer and additive concentration in the casting solution. Nanofiltration membranes are prepared using significantly lower concentrations of acid: 0.3 M HCl compared to the 2 M of either acetic or phosphoric acid used in previous works. It is shown that higher polymer concentrations can be used to prevent defect formation in the top layer. In addition, acetic acid concentration also strongly affects casting solution viscosity and thus can be used to control membrane structure, where lower acetic acid concentrations can prevent the formation of macrovoids in the support structure. The prepared nanofiltration membranes exhibit a very low molecular weight cutoff (210 ± 40 dalton), making these sustainable membranes very relevant for the removal of contaminants of emerging concern. Understanding how the parameters described here affect membrane preparation and performance is essential to optimizing membranes prepared with APS towards this important application.
    Language English
    Publishing date 2021-05-28
    Publishing country Switzerland
    Document type Journal Article
    ZDB-ID 2527146-5
    ISSN 2073-4360 ; 2073-4360
    ISSN (online) 2073-4360
    ISSN 2073-4360
    DOI 10.3390/polym13111775
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article ; Online: Tuning the charge of polyelectrolyte complex membranes prepared

    Durmaz, Elif Nur / Willott, Joshua D / Mizan, Md Mizanul Haque / de Vos, Wiebe M

    Soft matter

    2021  Volume 17, Issue 41, Page(s) 9420–9427

    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 ... ...

    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
    Language English
    Publishing date 2021-10-27
    Publishing country England
    Document type Journal Article
    ZDB-ID 2191476-X
    ISSN 1744-6848 ; 1744-683X
    ISSN (online) 1744-6848
    ISSN 1744-683X
    DOI 10.1039/d1sm01199e
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article: Tuning the structure and performance of polyelectrolyte complexation based aqueous phase separation membranes

    Baig, Muhammad Irshad / Willott, Joshua D / de Vos, Wiebe M

    Journal of membrane science. 2020 Dec. 01, v. 615

    2020  

    Abstract: Aqueous Phase Separation (APS) provides a new and sustainable platform to fabricate polymeric membranes entirely in water. Still, little is known on how the casting solution and coagulation bath compositions can be used to tune membrane structure and ... ...

    Abstract Aqueous Phase Separation (APS) provides a new and sustainable platform to fabricate polymeric membranes entirely in water. Still, little is known on how the casting solution and coagulation bath compositions can be used to tune membrane structure and performance. This work comprises a detailed investigation on the tuning parameters avaliable to tailor the morphology, pore size distribution, and water permeability of polyelectrolyte complex membranes prepared from poly(sodium 4-styrenesulfonate) (PSS) and polyallylamine hydrochloride (PAH). To avoid complexation of PAH and PSS in the casting solution, an optimum amount of base (NaOH) must be added to deprotonate PAH. In addition, the monomer mixing ratio of PSS to PAH significantly influences membrane morphology by modulating the interactions between the two polyelectrolytes. Coagulation bath pH can be used to control the driving force for complexation. Decreasing bath pH facilitates the formation of denser membranes, allowing ~97% protein retentions, whereas increasing bath pH leads to more open membrane structures. Changing the concentration of crosslinker in the coagulation bath allows tuning of membrane pore size from ~2 nm to ~46 nm, while simultaneously influencing membrane mechanical properties. Overall, this work highlights several key parameters to tune APS membrane morphology, demonstrating the versatility of APS to prepare optimized sustainable membranes for specific applications.
    Keywords artificial membranes ; coagulation ; electrolytes ; mechanical properties ; mixing ; mixing ratio ; pH ; permeability ; polyallylamines ; porosity ; separation ; sodium ; sodium hydroxide ; sulfonates
    Language English
    Dates of publication 2020-1201
    Publishing place Elsevier B.V.
    Document type Article
    ZDB-ID 194516-6
    ISSN 0376-7388
    ISSN 0376-7388
    DOI 10.1016/j.memsci.2020.118502
    Database NAL-Catalogue (AGRICOLA)

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  9. Article: Sustainable Aqueous Phase Separation membranes prepared through mild pH shift induced polyelectrolyte complexation of PSS and PEI

    Baig, Muhammad Irshad / Sari, Putu Putri Indira / Li, Jiaying / Willott, Joshua D / de Vos, Wiebe M

    Journal of membrane science. 2021 May 01, v. 625

    2021  

    Abstract: pH shift induced Aqueous phase separation (APS) is a novel and more sustainable water-based approach to create microfiltration, ultrafiltration, and nanofiltration membranes. APS allows for control over membrane pore size and structure in ways analogous ... ...

    Abstract pH shift induced Aqueous phase separation (APS) is a novel and more sustainable water-based approach to create microfiltration, ultrafiltration, and nanofiltration membranes. APS allows for control over membrane pore size and structure in ways analogous to traditional non-solvent induced phase separation (NIPS). Unfortunately, existing APS approaches require extreme pH shifts (from pH 14 to pH 1) to obtain successful membranes, limiting their applicability for large scale production. Here we demonstrate that APS membranes, with tunable pore sizes ranging from ~80 nm to dense nanofiltration type, can be prepared using a mild pH shift (pH 12 to pH 4) based on the complexation of poly(styrene sulfonate) (PSS) and branched polyethyleneimine (PEI) in acetate buffer coagulation baths. The molecular weight of PEI, the concentration and the pH value of the buffer solution, and the concentration of glutaraldehyde cross-linking agent were systematically varied to control and optimize the membrane fabrication conditions. It was found that tight nanofiltration membranes having a molecular weight cut-off of ~200 g mol⁻¹ and excellent salt (97% MgCl₂) and micropollutant retentions (~96%) could be prepared alongside ultra/microfiltration type membranes with an average pore size of ~60 nm. These results indicate that APS membranes with tunable pore sizes can be prepared under mild pH conditions with excellent control over separation properties.
    Keywords acetates ; coagulation ; cross-linking reagents ; electrolytes ; glutaraldehyde ; microfiltration ; molecular weight ; nanofiltration ; pH ; pollutants ; polyethyleneimine ; porosity ; separation ; styrene ; sulfonates ; ultrafiltration
    Language English
    Dates of publication 2021-0501
    Publishing place Elsevier B.V.
    Document type Article
    Note NAL-AP-2-clean
    ZDB-ID 194516-6
    ISSN 0376-7388
    ISSN 0376-7388
    DOI 10.1016/j.memsci.2021.119114
    Database NAL-Catalogue (AGRICOLA)

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  10. Article ; Online: Effect of surfactants on the thermoresponse of PNIPAM investigated in the brush geometry.

    Gresham, Isaac J / Willott, Joshua D / Johnson, Edwin C / Li, Peixun / Webber, Grant B / Wanless, Erica J / Nelson, Andrew R J / Prescott, Stuart W

    Journal of colloid and interface science

    2022  Volume 631, Issue Pt A, Page(s) 260–271

    Abstract: Hypothesis: Anionic surfactants have been reported to interact with poly(N-isopropyl acrylamide) (PNIPAM), suppressing its thermoresponse. Scattering and NMR studies of the anionic sodium dodecylsulfate (SDS) system propose that the PNIPAM-surfactant ... ...

    Abstract Hypothesis: Anionic surfactants have been reported to interact with poly(N-isopropyl acrylamide) (PNIPAM), suppressing its thermoresponse. Scattering and NMR studies of the anionic sodium dodecylsulfate (SDS) system propose that the PNIPAM-surfactant interaction is purely hydrophobic. However, prior phenomenological investigations of a range of surfactant identities (anionic, cationic, nonionic) show that only anionic surfactants affect the thermoresponse and conformation of PNIPAM, implying that the hydrophilic head-group also contributes. Crucially, the phenomenological experiments do not measure the affinity of the tested surfactants to the polymer, only their effect on its behaviour.
    Experiments: We study the adsorption of six surfactants within a planar PNIPAM brush system, elucidating the polymer conformation, thermoresponse, and surfactant adsorption kinetics using ellipsometry, neutron reflectometry (NR), optical reflectometry and the quartz crystal microbalance technique. NR is used to measure the distribution of surfactants within the brush.
    Findings: We find that only anionic surfactants modify the structure and thermoresponse of PNIPAM, with the greater affinity of anionic surfactants for PNIPAM (relative to cationic and nonionic surfactants) being the primary reason for this behaviour. These results show that the surfactant head-group has a more critical role in mediating PNIPAM-surfactant interaction than previously reported. Taking inspiration from prior molecular dynamics work on the PEO-surfactant system, we propose an interaction mechanism for PNIPAM and SDS that reconciles evidence for hydrophobic interaction with the observed head-group-dependent affinity.
    MeSH term(s) Surface-Active Agents ; Acrylic Resins ; Sodium Dodecyl Sulfate ; Pulmonary Surfactants ; Excipients ; Polymers
    Chemical Substances Surface-Active Agents ; poly-N-isopropylacrylamide (25189-55-3) ; Acrylic Resins ; Sodium Dodecyl Sulfate (368GB5141J) ; Pulmonary Surfactants ; Excipients ; Polymers
    Language English
    Publishing date 2022-10-25
    Publishing country United States
    Document type Journal Article
    ZDB-ID 241597-5
    ISSN 1095-7103 ; 0021-9797
    ISSN (online) 1095-7103
    ISSN 0021-9797
    DOI 10.1016/j.jcis.2022.10.071
    Database MEDical Literature Analysis and Retrieval System OnLINE

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