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  1. Article ; Online: Control over Charge Density by Tuning the Polyelectrolyte Type and Monomer Ratio in Saloplastic-Based Ion-Exchange Membranes.

    Krishna B, Ameya / de Vos, Wiebe M / Lindhoud, Saskia

    Langmuir : the ACS journal of surfaces and colloids

    2023  Volume 39, Issue 19, Page(s) 6874–6884

    Abstract: Membranes based on polyelectrolyte complexes (PECs) can now be prepared through several sustainable, organic solvent-free approaches. A recently developed approach allows PECs made by stoichiometric mixing of polyelectrolytes to be hot-pressed into dense ...

    Abstract Membranes based on polyelectrolyte complexes (PECs) can now be prepared through several sustainable, organic solvent-free approaches. A recently developed approach allows PECs made by stoichiometric mixing of polyelectrolytes to be hot-pressed into dense saloplastics, which then function as ion-exchange membranes. An important advantage of PECs is that tuning their properties can provide significant control over the properties of the fabricated materials, and thus over their separation properties. This work studies the effects of two key parameters─(a) ratio of mixing and (b) choice of polyelectrolytes─on the mechanical, material, and separation properties of their corresponding hot-pressed saloplastic-based ion-exchange membranes. By varying these two main parameters, charge density─the key property of any IEM─was found to be controllable. While studying several systems, including strong/strong, strong/weak, and weak/weak combinations of polyelectrolytes, it was observed that not all systems could be processed into saloplastic membranes. For the processable systems, expected trends were observed where a higher excess of one polyelectrolyte would lead to a more charged system, resulting in higher water uptake and better permselectivities. An anomaly was the polystyrenesulfonate-polyvinylamine system, which showed an opposite trend with a higher polycation ratio, leading to a more negative charge. Overall, we have found that it is possible to successfully fabricate saloplastic-based anion- and cation-exchange membranes with tunable charge densities through careful choice of polyelectrolyte combination and ratio of mixing.
    Language English
    Publishing date 2023-05-01
    Publishing country United States
    Document type Journal Article
    ZDB-ID 2005937-1
    ISSN 1520-5827 ; 0743-7463
    ISSN (online) 1520-5827
    ISSN 0743-7463
    DOI 10.1021/acs.langmuir.3c00497
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Fouling of nanofiltration membranes based on polyelectrolyte multilayers: The effect of a zwitterionic final layer

    Virga, Ettore / Žvab, Klara / de Vos, Wiebe M

    Journal of membrane science. 2021 Feb. 15, v. 620

    2021  

    Abstract: In this work, we investigate the effect of membrane surface chemistry on fouling in surface water treatment for polyelectrolyte multilayer based nanofiltration (NF) membranes. The polyelectrolyte multilayer approach allows us to prepare three membranes ... ...

    Abstract In this work, we investigate the effect of membrane surface chemistry on fouling in surface water treatment for polyelectrolyte multilayer based nanofiltration (NF) membranes. The polyelectrolyte multilayer approach allows us to prepare three membranes with the same active separation layer, apart from a difference in surface chemistry: nearly uncharged crosslinked Poly(allylamine hydrochloride) (PAH), strongly negative poly(sodium 4-styrene sulfonate) PSS and zwitterionic poly(2-methacryloyloxyethyl phosphorylcholine-co-acrylic acid) (PMPC-co-AA). Initially, we study foulant adsorption for the three different surfaces (on model interfaces), to demonstrate how a different surface chemistry of the top layer affects the subsequent adsorption of five different model foulants (Humic Acids, Alginates, Silica Nanoparticles, negatively and positively charged Proteins). Subsequently, we study fouling of the same model foulants on our polyelectrolyte multilayer based hollow fiber NF membranes with identical surface chemistry to the model surfaces. Our results show that nearly uncharged crosslinked PAH surface generally fouls more than strongly negatively charged PSS surface. While negative BSA adsorbs better on PSS, probably due to charge regulation. Overall, fouling was mainly driven by electrostatic and acid-base interactions, which led, for both PAH and PSS terminated membranes, to flux decline and changes in selectivity. In contrast, we demonstrate through filtration experiments carried out with synthetic and real surface water, that the bio-inspired zwitterionic phosphatidylcholine surface chemistry exhibits excellent fouling resistance and thus stable performance during filtration.
    Keywords adsorption ; alginates ; crosslinking ; nanofiltration ; phosphatidylcholines ; silica ; sodium ; sulfonates ; surface water ; water treatment ; zwitterions
    Language English
    Dates of publication 2021-0215
    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.2020.118793
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  3. Article: Advanced Oxidation Processes Coupled to Nanofiltration Membranes with Catalytic Fe

    Wang, Tao / Bachs, Enrique Serra / de Grooth, Joris / de Vos, Wiebe M

    Membranes

    2023  Volume 13, Issue 4

    Abstract: The in situ synthesis of ... ...

    Abstract The in situ synthesis of Fe
    Language English
    Publishing date 2023-03-28
    Publishing country Switzerland
    Document type Journal Article
    ZDB-ID 2614641-1
    ISSN 2077-0375
    ISSN 2077-0375
    DOI 10.3390/membranes13040388
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  4. Article ; Online: Combined Electrospinning-Electrospraying for High-Performance Bipolar Membranes with Incorporated MCM-41 as Water Dissociation Catalysts.

    Al-Dhubhani, Emad / Tedesco, Michele / de Vos, Wiebe M / Saakes, Michel

    ACS applied materials & interfaces

    2023  Volume 15, Issue 39, Page(s) 45745–45755

    Abstract: Electrospinning has been demonstrated as a very promising method to create bipolar membranes (BPMs), especially as it allows three-dimensional (3D) junctions of entangled anion exchange and cation exchange nanofibers. These newly developed BPMs are ... ...

    Abstract Electrospinning has been demonstrated as a very promising method to create bipolar membranes (BPMs), especially as it allows three-dimensional (3D) junctions of entangled anion exchange and cation exchange nanofibers. These newly developed BPMs are relevant to demanding applications, including acid and base production, fuel cells, flow batteries, ammonia removal, concentration of carbon dioxide, and hydrogen generation. However, these applications require the introduction of catalysts into the BPM to allow accelerated water dissociation, and this remains a challenge. Here, we demonstrate a versatile strategy to produce very efficient BPMs through a combined electrospinning-electrospraying approach. Moreover, this work applies the newly investigated water dissociation catalyst of nanostructured silica MCM-41. Several BPMs were produced by electrospraying MCM-41 nanoparticles into the layers directly adjacent to the main BPM 3D junction. BPMs with various loadings of MCM-41 nanoparticles and BPMs with different catalyst positions relative to the junction were investigated. The membranes were carefully characterized for their structure and performance. Interestingly, the water dissociation performance of BPMs showed a clear optimal MCM-41 loading where the performance outpaced that of a commercial BPM, recording a transmembrane voltage of approximately 1.11 V at 1000 A/m
    Language English
    Publishing date 2023-09-20
    Publishing country United States
    Document type Journal Article
    ISSN 1944-8252
    ISSN (online) 1944-8252
    DOI 10.1021/acsami.3c06826
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Fouling of polyelectrolyte multilayer based nanofiltration membranes during produced water treatment: The role of surfactant size and chemistry.

    Virga, Ettore / Parra, Mario Alejandro / de Vos, Wiebe M

    Journal of colloid and interface science

    2021  Volume 594, Page(s) 9–19

    Abstract: Large volumes of water become contaminated with hydrocarbons, surfactants, salts and other chemical agents during Oil & Gas exploration activities, resulting in a complex wastewater stream known as produced water (PW). Nanofiltration (NF) membranes are a ...

    Abstract Large volumes of water become contaminated with hydrocarbons, surfactants, salts and other chemical agents during Oil & Gas exploration activities, resulting in a complex wastewater stream known as produced water (PW). Nanofiltration (NF) membranes are a promising alternative for the treatment of PW to facilitate its re-use. Unfortunately, membrane fouling still represents a major obstacle. In the present work, we investigate the effect of surface chemistry on fouling of NF membranes based on polyelectrolyte multilayers (PEM), during the treatment of artificial produced water. To this end, oil-in-water (O/W) emulsions stabilized with four different surfactants (anionic, cationic, zwitterionic and non-ionic) were treated with PEM-based NF membranes having the same multilayer, but different top layer polymer chemistry: crosslinked poly(allylamine hydrochloride) (PAH, nearly uncharged), poly(sodium 4-styrene sulfonate) (PSS, strongly negative), poly(sulfobetaine methacrylate-co-acrylic acid) (PSBMA-co-AA, zwitterionic) and Nafion (negative and hydrophobic). First, we study the adsorption of the four surfactants for the four different surfaces on model interfaces. Second, we study fouling by artificial produced water stabilized by the same surfactants on PEM-based hollow fiber NF membranes characterized by the same multilayer of our model surfaces. Third, we study fouling of the same surfactants solution but without oil. Very high oil retention (>99%) was observed when filtering all the O/W emulsions, while the physicochemical interactions between the multilayer and the surfactants determined the extent of fouling as well as the surfactant retention. Unexpectedly, our results show that fouling of PEM-based NF membranes, during PW treatment, is mainly due to membrane active layer fouling caused by surfactant uptake inside of the PEM coating, rather than due to cake layer formation. Indeed, it is not the surface chemistry of the membrane that determines the extent of fouling, but the surfactant interaction with the bulk of the PEM. A denser multilayer, that would stop these molecules, would benefit PW treatment by decreasing fouling issues, as would the use of slightly more bulky surfactants that cannot penetrate the PEM.
    Language English
    Publishing date 2021-03-09
    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.2021.02.119
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article: Biocatalytic membranes through aqueous phase separation

    van Lente, Jéré J. / Baig, M. Irshad / de Vos, Wiebe M. / Lindhoud, Saskia

    Journal of colloid and interface science. 2022 June 15, v. 616

    2022  

    Abstract: Test Polymer membranes play a critical role in water treatment, chemical industry, and medicine. Unfortunately, the current standard for polymer membrane production requires unsustainable and harmful organic solvents. Aqueous phase separation (APS) has ... ...

    Abstract Test Polymer membranes play a critical role in water treatment, chemical industry, and medicine. Unfortunately, the current standard for polymer membrane production requires unsustainable and harmful organic solvents. Aqueous phase separation (APS) has recently been proposed as a method to produce membranes in a more sustainable manner through induced polyelectrolyte complexation in aqueous solutions. We demonstrate that APS has another natural advantage that goes beyond sustainability: the easy incorporation of enzymes in the membrane structure. Biocatalytic membranes hold great promise in for example biorefinery, but the most common current post-production processes to immobilize enzymes on the membrane surface are complicated and expensive. In this study we demonstrated the first biocatalytic membrane produced via APS. We demonstrate an easy procedure to incorporate lysozyme in polyelectrolyte complex membranes made via APS. Our functionalized membranes have the same structure, water permeability (in the range of high nanofiltration, low ultrafiltration), and retention as membranes without lysozyme. Lysozyme is antibacterial by catalysing the hydrolysis of specific peptidoglycan bonds in bacteria walls. We demonstrate that the functionalized membranes are also capable of catalysing this reaction. The membranes remain enzymatically active for a period of at least one week. This opens new routes to produce polymer membranes with added biological function.
    Keywords biorefining ; chemical industry ; electrolytes ; hydrolysis ; lysozyme ; medicine ; nanofiltration ; peptidoglycans ; permeability ; polymers ; separation ; ultrafiltration ; water treatment
    Language English
    Dates of publication 2022-0615
    Size p. 903-910.
    Publishing place Elsevier Inc.
    Document type Article
    ZDB-ID 241597-5
    ISSN 1095-7103 ; 0021-9797
    ISSN (online) 1095-7103
    ISSN 0021-9797
    DOI 10.1016/j.jcis.2022.02.094
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  7. Article: Theory of Oil Fouling for Microfiltration and Ultrafiltration Membranes in Produced Water Treatment

    Virga, Ettore / Field, Robert W. / Biesheuvel, P.M. / de Vos, Wiebe M.

    Journal of colloid and interface science. 2022 Apr. 06,

    2022  

    Abstract: Due to the complexity of oil-in-water emulsions, the existing literature is still missing a mathematical tool that can describe membrane fouling in a fully quantitative manner on the basis of relevant fouling mechanisms. In this work, a quantitative ... ...

    Abstract Due to the complexity of oil-in-water emulsions, the existing literature is still missing a mathematical tool that can describe membrane fouling in a fully quantitative manner on the basis of relevant fouling mechanisms. In this work, a quantitative model that successfully describes cake layer formation and pore blocking is presented. We propose that the degree of pore blocking is determined by the membrane contact angle and the resulting surface coverage, while the cake layer is described by a mass balance and a cake erosion flux. The model is validated by comparison to experimental data from previous works [1,2] where membrane type, surfactant type and salinity were varied. Most input parameters could be directly taken from the experimental conditions, while four fitting parameters were required. The experimental data can be well described by the model which was developed to provide insight into the dominant fouling mechanisms. Moreover, where existing models usually assume that pore blocking precedes cake layer formation, here we find that cake layer formation can start and occur while the degree of pore blocking is still increasing, in line with the more dynamic nature of oil droplets filtration. These new conceptual advances in the field of colloid and interface science open up new pathways for membrane fouling understanding, prevention and control.
    Keywords cakes ; contact angle ; microfiltration ; models ; oils ; salinity ; surfactants ; ultrafiltration ; water treatment
    Language English
    Dates of publication 2022-0406
    Publishing place Elsevier Inc.
    Document type Article
    Note Pre-press version
    ZDB-ID 241597-5
    ISSN 1095-7103 ; 0021-9797
    ISSN (online) 1095-7103
    ISSN 0021-9797
    DOI 10.1016/j.jcis.2022.04.039
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  8. Article: Sustainable K+/Na+ monovalent-selective membranes with hot-pressed PSS-PVA saloplastics

    Krishna B, Ameya / Zwijnenberg, Harmen J. / Lindhoud, Saskia / de Vos, Wiebe M.

    Journal of membrane science. 2022 June 15, v. 652

    2022  

    Abstract: Monovalent selective cation exchange membranes could play an important role in balancing the K⁺/Na⁺ ratio in agricultural feed streams to prevent the toxic effects of excess Na⁺ in the plant and soil systems, especially in greenhouses and dry areas. A ... ...

    Abstract Monovalent selective cation exchange membranes could play an important role in balancing the K⁺/Na⁺ ratio in agricultural feed streams to prevent the toxic effects of excess Na⁺ in the plant and soil systems, especially in greenhouses and dry areas. A polyelectrolyte complex of polystyrenesulfonate and polyvinylamine in the monomer ratio 1:2.5 is hot-pressed to form a dense saloplastic. The plastic takes up 42% w/w water when equilibrated, while ion-exchange capacity measurements show that it is negatively charged with a net ion-exchange capacity of 1.1 ± 0.4. Resistance measurements show a very promising preferred conductivity for K⁺ over Na⁺. This was confirmed by measuring K⁺ and Na⁺ transport through the membrane under diffusive conditions from an aqueous mixture of KCl and NaCl. Commercial membranes show resistance-based selectivities of 1.32 ± 0.1 to 1.19 ± 0.1, and diffusion based selectivities of 0.99 ± 0.1 to 0.78 ± 0.1. In contrast, the selectivities for the newly developed saloplastic membrane were 1.80 ± 0.33 for the resistance-based selectivity while the diffusion-based selectivity was 1.91 ± 0.1. The procedure is green as toxic solvents and/or halogenating agents, typically used to make cation exchange membranes, are not needed. This work thus highlights how monovalent selective membranes with a relevant K⁺/Na⁺ selectivity can be prepared by a simple and sustainable hot-pressing approach.
    Keywords cation exchange ; electrolytes ; ion exchange capacity ; plastics ; soil ; toxicity
    Language English
    Dates of publication 2022-0615
    Publishing place Elsevier B.V.
    Document type Article
    ZDB-ID 194516-6
    ISSN 0376-7388
    ISSN 0376-7388
    DOI 10.1016/j.memsci.2022.120463
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  9. Article: CoFe2O4-peroxymonosulfate based catalytic UF and NF polymeric membranes for naproxen removal: The role of residence time

    Wang, Tao / de Vos, Wiebe M. / de Grooth, Joris

    Journal of membrane science. 2022 Mar. 15, v. 646

    2022  

    Abstract: Micropollutants pose a significant threat to water quality, aquatic life, and public health. A catalytic polymeric membrane, combining membrane filtration and peroxymonosulfate (PMS) activation provides an alternative option to their treatment. In this ... ...

    Abstract Micropollutants pose a significant threat to water quality, aquatic life, and public health. A catalytic polymeric membrane, combining membrane filtration and peroxymonosulfate (PMS) activation provides an alternative option to their treatment. In this work, CoFe₂O₄ based catalytic particles were blended with polyethersulfone (PES) polymer and catalytic UF (ultrafiltration) membranes were fabricated by non-solvent induced phase inversion. The catalytic UF membrane with 2.0% CoFe₂O₄ concentration can effectively degrade 70% naproxen in a batch experiment. Additionally, a stable selective layer was built by the layer-by-layer assembly of PDADMAC (poly(diallyldimethylammonium chloride)) and PSS (poly(styrenesulfonate)) on the surface of the catalytic UF membrane. Both the catalytic UF and NF (nanofiltration) membranes were measured in full-recycling mode and single-pass mode. In the full-recycling mode, the naproxen rejection of catalytic UF and NF membranes both increased after adding PMS due to the activation of PMS and increased adsorption. Naproxen removal at different fluxes indicates that longer residence time (i.e. lower flux) can effectively decrease the naproxen concentration in the permeate. The same effect of residence time was also observed in the single-pass mode. By prolonging the residence time of UF membranes to the same level of the NF membranes, the catalytic UF membrane exhibited 87.7% naproxen rejection which is comparable to that of the NF membranes. Significantly, the pressure used in the UF membrane was only 0.1 bar, showing a great advantage of reduced energy cost. These results reveal the important role of residence time on the treatment efficiency of micropollutants by catalytic membranes. Moreover, the application of catalytic UF membranes under low pressure provides an energy-friendly way of removing micropollutants.
    Keywords adsorption ; aquatic organisms ; chlorides ; energy costs ; microfiltration ; nanofiltration ; pollutants ; polymers ; public health ; ultrafiltration ; water quality
    Language English
    Dates of publication 2022-0315
    Publishing place Elsevier B.V.
    Document type Article
    ZDB-ID 194516-6
    ISSN 0376-7388
    ISSN 0376-7388
    DOI 10.1016/j.memsci.2021.120209
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  10. 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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