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Membranes
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Mixed Matrix Membranes
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Mixed Matrix Membranes

A special issue of Membranes (ISSN 2077-0375). This special issue belongs to the section "Membrane Analysis and Characterization".

Deadline for manuscript submissions: closed (15 May 2018) | Viewed by 42697

Printed Edition Available!
A printed edition of this Special Issue is available here.

Special Issue Editor

Dr. Clara Casado-Coterillo

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Guest Editor
Department of Chemical and Biomolecular Engineering, University of Cantabria, Av. Los Castros s/n, 39005 Santander, Spain
Interests: synthesis; characterization; CO2 capture and utilization; mixed matrix membranes; pervaporation; sustainable process intensification using membranes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

This Special Issue, entitled “Mixed Matrix Membranes”, is motivated by the gap between growing interest in developing novel mixed matrix membranes by various research groups and the lack of large-scale implementation. This includes important issues regarding fabrication, such as compatibility and adhesion, fabrication (solution casting, dip-coating, spinning, interfacial polymerization, layer-by-layer, etc.), configuration, geometry (flat-sheet, hollow fiber, composite, asymmetric), post-treatment, types of additives/fillers (zeolites, ionic liquids, ion-exchange materials, layered porous materials, MOFs, etc.), and reproducibility, membrane characterization (e.g., chemical, structural, morphological, electrical, compositional, mechanical and topographical properties, as well as membrane transport and separation), and applications of membranes in different fields, especially in CO2 separation from other gases, with a special focus on the influence of impurities, such as water vapor and ion exchange membranes for several electrochemical devices, such as innovative energy storage systems. Overall, this Special Issue is orientated to all the above-cited research topics, directed to the advancement of mixed matrix membranes and novel materials in membrane technology to solve some of the environmental and technical challenges faced by chemical industries.

Dr. Clara Casado Coterillo
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Membranes is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2200 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Membrane fabrication
  • Membrane modification
  • Characterization techniques
  • Flat-sheet membrane
  • Hollow fiber membrane
  • Spinning
  • Filler dispersion
  • Interfacial polymerization
  • Compatibility
  • Gas separation
  • Ion exchange membranes
  • Ion exchange capacity
  • Water vapour

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Related Special Issue

Published Papers (11 papers)

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Editorial

Jump to: Research, Review

5 pages, 207 KiB  
Editorial
Mixed Matrix Membranes
by Clara Casado-Coterillo
Membranes 2019, 9(11), 149; https://doi.org/10.3390/membranes9110149 - 10 Nov 2019
Cited by 21 | Viewed by 4235
Abstract
In recent decades, mixed matrix membranes (MMMs) have attracted considerable interest in research laboratories worldwide, motivated by the gap between the growing interest in developing novel mixed matrix membranes by various research groups and the lack of large-scale implementation. This Special Issue contains [...] Read more.
In recent decades, mixed matrix membranes (MMMs) have attracted considerable interest in research laboratories worldwide, motivated by the gap between the growing interest in developing novel mixed matrix membranes by various research groups and the lack of large-scale implementation. This Special Issue contains six publications dealing with the current opportunities and challenges of mixed matrix membranes development and applications as solutions for the environmental and health challenges of 21st century society. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)

Research

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24 pages, 3713 KiB  
Article
Superglassy Polymers to Treat Natural Gas by Hybrid Membrane/Amine Processes: Can Fillers Help?
by Ahmed W. Ameen, Peter M. Budd and Patricia Gorgojo
Membranes 2020, 10(12), 413; https://doi.org/10.3390/membranes10120413 - 10 Dec 2020
Cited by 10 | Viewed by 3708
Abstract
Superglassy polymers have emerged as potential membrane materials for several gas separation applications, including acid gas removal from natural gas. Despite the superior performance shown at laboratory scale, their use at industrial scale is hampered by their large drop in gas permeability over [...] Read more.
Superglassy polymers have emerged as potential membrane materials for several gas separation applications, including acid gas removal from natural gas. Despite the superior performance shown at laboratory scale, their use at industrial scale is hampered by their large drop in gas permeability over time due to physical aging. Several strategies are proposed in the literature to prevent loss of performance, the incorporation of fillers being a successful approach. In this work, we provide a comprehensive economic study on the application of superglassy membranes in a hybrid membrane/amine process for natural gas sweetening. The hybrid process is compared with the more traditional stand-alone amine-absorption technique for a range of membrane gas separation properties (CO2 permeance and CO2/CH4 selectivity), and recommendations for long-term membrane performance are made. These recommendations can drive future research on producing mixed matrix membranes (MMMs) of superglassy polymers with anti-aging properties (i.e., target permeance and selectivity is maintained over time), as thin film nanocomposite membranes (TFNs). For the selected natural gas composition of 28% of acid gas content (8% CO2 and 20% H2S), we have found that a CO2 permeance of 200 GPU and a CO2/CH4 selectivity of 16 is an optimal target. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes II. From Lab Scale towards Application)
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20 pages, 2681 KiB  
Article
Energy Storage Behavior of Lithium-Ion Conducting poly(vinyl alcohol) (PVA): Chitosan(CS)-Based Polymer Blend Electrolyte Membranes: Preparation, Equivalent Circuit Modeling, Ion Transport Parameters, and Dielectric Properties
by Mohamad Brza, Shujahadeen B. Aziz, Salah Raza Saeed, Muhamad H. Hamsan, Siti Rohana Majid, Rebar T. Abdulwahid, Mohd F. Z. Kadir and Ranjdar M. Abdullah
Membranes 2020, 10(12), 381; https://doi.org/10.3390/membranes10120381 - 30 Nov 2020
Cited by 24 | Viewed by 3214
Abstract
Plasticized lithium-ion-based-conducting polymer blend electrolytes based on poly(vinyl alcohol) (PVA):chitosan (CS) polymer was prepared using a solution cast technique. The conductivity of the polymer electrolyte system was found to be 8.457 × 10−4 S/cm, a critical factor for electrochemical device applications. It [...] Read more.
Plasticized lithium-ion-based-conducting polymer blend electrolytes based on poly(vinyl alcohol) (PVA):chitosan (CS) polymer was prepared using a solution cast technique. The conductivity of the polymer electrolyte system was found to be 8.457 × 10−4 S/cm, a critical factor for electrochemical device applications. It is indicated that the number density (n), diffusion coefficient (D), and mobility (μ) of ions are increased with the concentration of glycerol. High values of dielectric constant and dielectric loss were observed at low frequency region. A correlation was found between the dielectric constant and DC conductivity. The achieved transference number of ions (tion) and electrons (te) for the highest conducting plasticized sample were determined to be 0.989 and 0.011, respectively. The electrochemical stability for the highest conducting sample was 1.94 V, indicated by linear sweep voltammetry (LSV). The cyclic voltammetry (CV) response displayed no redox reaction peaks through its entire potential range. Through the constructing electric double-layer capacitor, the energy storage capacity of the highest conducting sample was investigated. All decisive parameters of the EDLC were determined. At the first cycle, the specific capacitance, internal resistance, energy density, and power density were found to be 130 F/g, 80 Ω, 14.5 Wh/kg, and 1100 W/kg, respectively. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes II. From Lab Scale towards Application)
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17 pages, 5259 KiB  
Article
Magnetically Aligned and Enriched Pathways of Zeolitic Imidazolate Framework 8 in Matrimid Mixed Matrix Membranes for Enhanced CO2 Permeability
by Machiel van Essen, Esther Montrée, Menno Houben, Zandrie Borneman and Kitty Nijmeijer
Membranes 2020, 10(7), 155; https://doi.org/10.3390/membranes10070155 - 17 Jul 2020
Cited by 14 | Viewed by 3853
Abstract
Metal-organic frameworks (MOFs) as additives in mixed matrix membranes (MMMs) for gas separation have gained significant attention over the past decades. Many design parameters have been investigated for MOF based MMMs, but the spatial distribution of the MOF throughout MMMs lacks investigation. Therefore, [...] Read more.
Metal-organic frameworks (MOFs) as additives in mixed matrix membranes (MMMs) for gas separation have gained significant attention over the past decades. Many design parameters have been investigated for MOF based MMMs, but the spatial distribution of the MOF throughout MMMs lacks investigation. Therefore, magnetically aligned and enriched pathways of zeolitic imidazolate framework 8 (ZIF−8) in Matrimid MMMs were synthesized and investigated by means of their N2 and CO2 permeability. Magnetic ZIF−8 (m–ZIF−8) was synthesized by incorporating Fe3O4 in the ZIF−8 structure. The presence of Fe3O4 in m–ZIF−8 showed a decrease in surface area and N2 and CO2 uptake, with respect to pure ZIF−8. Alignment of m–ZIF−8 in Matrimid showed the presence of enriched pathways of m–ZIF−8 through the MMMs. At 10 wt.% m–ZIF−8 incorporation, no effect of alignment was observed for the N2 and CO2 permeability, which was ascribed anon-ideal tortuous alignment. However, alignment of 20 wt.% m–ZIF−8 in Matrimid showed to increase the CO2 diffusivity and permeability (19%) at 7 bar, while no loss in ideal selectivity was observed, with respect to homogeneously dispersed m–ZIF−8 membranes. Thus, the alignment of MOF particles throughout the matrix was shown to enhance the CO2 permeability at a certain weight content of MOF. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes II. From Lab Scale towards Application)
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17 pages, 3770 KiB  
Article
Exploring the Gas-Permeation Properties of Proton-Conducting Membranes Based on Protic Imidazolium Ionic Liquids: Application in Natural Gas Processing
by Parashuram Kallem, Christophe Charmette, Martin Drobek, Anne Julbe, Reyes Mallada and Maria Pilar Pina
Membranes 2018, 8(3), 75; https://doi.org/10.3390/membranes8030075 - 5 Sep 2018
Cited by 5 | Viewed by 5265
Abstract
This experimental study explores the potential of supported ionic liquid membranes (SILMs) based on protic imidazolium ionic liquids (ILs) and randomly nanoporous polybenzimidazole (PBI) supports for CH4/N2 separation. In particular, three classes of SILMs have been prepared by the infiltration [...] Read more.
This experimental study explores the potential of supported ionic liquid membranes (SILMs) based on protic imidazolium ionic liquids (ILs) and randomly nanoporous polybenzimidazole (PBI) supports for CH4/N2 separation. In particular, three classes of SILMs have been prepared by the infiltration of porous PBI membranes with different protic moieties: 1-H-3-methylimidazolium bis (trifluoromethane sulfonyl)imide; 1-H-3-vinylimidazolium bis(trifluoromethane sulfonyl)imide followed by in situ ultraviolet (UV) polymerization to poly[1-(3H-imidazolium)ethylene] bis(trifluoromethanesulfonyl)imide. The polymerization process has been monitored by Fourier transform infrared (FTIR) spectroscopy and the concentration of the protic entities in the SILMs has been evaluated by thermogravimetric analysis (TGA). Single gas permeability values of N2 and CH4 at 313 K, 333 K and 363 K were obtained from a series of experiments conducted in a batch gas permeance system. The results obtained were assessed in terms of the preferential cavity formation and favorable solvation of methane in the apolar domains of the protic ionic network. The most attractive behavior exhibited poly[1-(3H-imidazolium)ethylene]bis(trifluoromethanesulfonyl)imide polymeric ionic liquid (PIL) cross-linked with 1% divinylbenzene supported membranes, showing stable performance when increasing the upstream pressure. The CH4/N2 permselectivity value of 2.1 with CH4 permeability of 156 Barrer at 363 K suggests that the transport mechanism of the as-prepared SILMs is solubility-dominated. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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15 pages, 4209 KiB  
Article
Estimating CO2/N2 Permselectivity through Si/Al = 5 Small-Pore Zeolites/PTMSP Mixed Matrix Membranes: Influence of Temperature and Topology
by Clara Casado-Coterillo, Ana Fernández-Barquín, Susana Valencia and Ángel Irabien
Membranes 2018, 8(2), 32; https://doi.org/10.3390/membranes8020032 - 16 Jun 2018
Cited by 10 | Viewed by 4022
Abstract
In the present work, the effect of zeolite type and topology on CO2 and N2 permeability using zeolites of different topology (CHA, RHO, and LTA) in the same Si/Al = 5, embedded in poly(trimethylsilyl-1-propyne) (PTMSP) is evaluated with temperature. Several models [...] Read more.
In the present work, the effect of zeolite type and topology on CO2 and N2 permeability using zeolites of different topology (CHA, RHO, and LTA) in the same Si/Al = 5, embedded in poly(trimethylsilyl-1-propyne) (PTMSP) is evaluated with temperature. Several models are compared on the prediction of CO2/N2 separation performance and then the modified Maxwell models are selected. The CO2 and N2 permeabilities through these membranes are predicted with an average absolute relative error (AARE) lower than 0.6% taking into account the temperature and zeolite loading and topology on non-idealities such as membrane rigidification, zeolite–polymer compatibility and sieve pore blockage. The evolution of this structure–performance relationship with temperature has also been predicted. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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17 pages, 4624 KiB  
Article
CO2 Separation in Nanocomposite Membranes by the Addition of Amidine and Lactamide Functionalized POSS® Nanoparticles into a PVA Layer
by Gabriel Guerrero, May-Britt Hägg, Christian Simon, Thijs Peters, Nicolas Rival and Christelle Denonville
Membranes 2018, 8(2), 28; https://doi.org/10.3390/membranes8020028 - 8 Jun 2018
Cited by 17 | Viewed by 4339
Abstract
In this article, we studied two different types of polyhedral oligomeric silsesquioxanes (POSS®) functionalized nanoparticles as additives for nanocomposite membranes for CO2 separation. One with amidine functionalization (Amidino POSS®) and the second with amine and lactamide groups functionalization [...] Read more.
In this article, we studied two different types of polyhedral oligomeric silsesquioxanes (POSS®) functionalized nanoparticles as additives for nanocomposite membranes for CO2 separation. One with amidine functionalization (Amidino POSS®) and the second with amine and lactamide groups functionalization (Lactamide POSS®). Composite membranes were produced by casting a polyvinyl alcohol (PVA) layer, containing either amidine or lactamide functionalized POSS® nanoparticles, on a polysulfone (PSf) porous support. FTIR characterization shows a good compatibility between the nanoparticles and the polymer. Differential scanning calorimetry (DSC) and the dynamic mechanical analysis (DMA) show an increment of the crystalline regions. Both the degree of crystallinity (Xc) and the alpha star transition, associated with the slippage between crystallites, increase with the content of nanoparticles in the PVA selective layer. These crystalline regions were affected by the conformation of the polymer chains, decreasing the gas separation performance. Moreover, lactamide POSS® shows a higher interaction with PVA, inducing lower values in the CO2 flux. We have concluded that the interaction of the POSS® nanoparticles increased the crystallinity of the composite membranes, thereby playing an important role in the gas separation performance. Moreover, these nanocomposite membranes did not show separation according to a facilitated transport mechanism as expected, based on their functionalized amino-groups, thus, solution-diffusion was the main mechanism responsible for the transport phenomena. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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14 pages, 2409 KiB  
Article
Hydrolytic Degradation and Mechanical Stability of Poly(ε-Caprolactone)/Reduced Graphene Oxide Membranes as Scaffolds for In Vitro Neural Tissue Regeneration
by Sandra Sánchez-González, Nazely Diban and Ane Urtiaga
Membranes 2018, 8(1), 12; https://doi.org/10.3390/membranes8010012 - 5 Mar 2018
Cited by 75 | Viewed by 5749
Abstract
The present work studies the functional behavior of novel poly(ε-caprolactone) (PCL) membranes functionalized with reduced graphene oxide (rGO) nanoplatelets under simulated in vitro culture conditions (phosphate buffer solution (PBS) at 37 °C) during 1 year, in order to elucidate their applicability as scaffolds [...] Read more.
The present work studies the functional behavior of novel poly(ε-caprolactone) (PCL) membranes functionalized with reduced graphene oxide (rGO) nanoplatelets under simulated in vitro culture conditions (phosphate buffer solution (PBS) at 37 °C) during 1 year, in order to elucidate their applicability as scaffolds for in vitro neural regeneration. The morphological, chemical, and DSC results demonstrated that high internal porosity of the membranes facilitated water permeation and procured an accelerated hydrolytic degradation throughout the bulk pathway. Therefore, similar molecular weight reduction, from 80 kDa to 33 kDa for the control PCL, and to 27 kDa for PCL/rGO membranes, at the end of the study, was observed. After 1 year of hydrolytic degradation, though monomers coming from the hydrolytic cleavage of PCL diffused towards the PBS medium, the pH was barely affected, and the rGO nanoplatelets mainly remained in the membranes which envisaged low cytotoxic effect. On the other hand, the presence of rGO nanomaterials accelerated the loss of mechanical stability of the membranes. However, it is envisioned that the gradual degradation of the PCL/rGO membranes could facilitate cells infiltration, interconnectivity, and tissue formation. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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18 pages, 6132 KiB  
Article
Mixed Matrix Membranes of Boron Icosahedron and Polymers of Intrinsic Microporosity (PIM-1) for Gas Separation
by Muntazim Munir Khan, Sergey Shishatskiy and Volkan Filiz
Membranes 2018, 8(1), 1; https://doi.org/10.3390/membranes8010001 - 2 Jan 2018
Cited by 24 | Viewed by 8176
Abstract
This work reports on the preparation and gas transport performance of mixed matrix membranes (MMMs) based on the polymer of intrinsic microporosity (PIM-1) and potassium dodecahydrododecaborate (K2B12H12) as inorganic particles (IPs). The effect of IP loading on [...] Read more.
This work reports on the preparation and gas transport performance of mixed matrix membranes (MMMs) based on the polymer of intrinsic microporosity (PIM-1) and potassium dodecahydrododecaborate (K2B12H12) as inorganic particles (IPs). The effect of IP loading on the gas separation performance of these MMMs was investigated by varying the IP content (2.5, 5, 10 and 20 wt %) in a PIM-1 polymer matrix. The derived MMMs were characterized by scanning electron microscopy (SEM), thermogravimetric analysis (TGA), single gas permeation tests and sorption measurement. The PIM1/K2B12H12 MMMs show good dispersion of the IPs (from 2.5 to 10 wt %) in the polymer matrix. The gas permeability of PIM1/K2B12H12 MMMs increases as the loading of IPs increases (up to 10 wt %) without sacrificing permselectivity. The sorption isotherm in PIM-1 and PIM1/K2B12H12 MMMs demonstrate typical dual-mode sorption behaviors for the gases CO2 and CH4. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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Review

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31 pages, 5692 KiB  
Review
Metal Organic Framework Based Polymer Mixed Matrix Membranes: Review on Applications in Water Purification
by Asmaa Elrasheedy, Norhan Nady, Mohamed Bassyouni and Ahmed El-Shazly
Membranes 2019, 9(7), 88; https://doi.org/10.3390/membranes9070088 - 19 Jul 2019
Cited by 113 | Viewed by 10662
Abstract
Polymeric membranes have been widely employed for water purification applications. However, the trade-off issue between the selectivity and permeability has limited its use in various applications. Mixed matrix membranes (MMMs) were introduced to overcome this limitation and to enhance the properties and performance [...] Read more.
Polymeric membranes have been widely employed for water purification applications. However, the trade-off issue between the selectivity and permeability has limited its use in various applications. Mixed matrix membranes (MMMs) were introduced to overcome this limitation and to enhance the properties and performance of polymeric membranes by incorporation of fillers such as silica and zeolites. Metal-organic frameworks (MOFs) are a new class of hybrid inorganic–organic materials that are introduced as novel fillers for incorporation in polymeric matrix to form composite membranes for different applications especially water desalination. A major advantage of MOFs over other inorganic fillers is the possibility of preparing different structures with different pore sizes and functionalities, which are designed especially for a targeted application. Different MMMs fabrication techniques have also been investigated to fabricate MMMs with pronounced properties for a specific application. Synthesis techniques include blending, layer-by-layer (LBL), gelatin-assisted seed growth and in situ growth that proved to give the most homogenous dispersion of MOFs within the organic matrix. It was found that the ideal filler loading of MOFs in different polymeric matrices is 10%, increasing the filler loading beyond this value led to formation of aggregates that significantly decreased the MOFs-MMMs performance. Despite the many merits of MOFs-MMMs, the main challenge facing the upscaling and wide commercial application of MOFs-MMMs is the difficult synthesis conditions of the MOFs itself and the stability and sustainability of MOFs-MMMs performance. Investigation of new MOFs and MOFs-MMMs synthesis techniques should be carried out for further industrial applications. Among these new synthesis methods, green MOFs synthesis has been highlighted as low cost, renewable, environmentally friendly and recyclable starting materials for MOFs-MMMs. This paper will focus on the investigation of the effect of different recently introduced MOFs on the performance of MOFs-MMMs in water purification applications. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes II. From Lab Scale towards Application)
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48 pages, 5810 KiB  
Review
Performance of Mixed Matrix Membranes Containing Porous Two-Dimensional (2D) and Three-Dimensional (3D) Fillers for CO2 Separation: A Review
by Mahdi Ahmadi, Saravanan Janakiram, Zhongde Dai, Luca Ansaloni and Liyuan Deng
Membranes 2018, 8(3), 50; https://doi.org/10.3390/membranes8030050 - 28 Jul 2018
Cited by 70 | Viewed by 9346
Abstract
Application of conventional polymeric membranes in CO2 separation processes are limited by the existing trade-off between permeability and selectivity represented by the renowned upper bound. Addition of porous nanofillers in polymeric membranes is a promising approach to transcend the upper bound, owing [...] Read more.
Application of conventional polymeric membranes in CO2 separation processes are limited by the existing trade-off between permeability and selectivity represented by the renowned upper bound. Addition of porous nanofillers in polymeric membranes is a promising approach to transcend the upper bound, owing to their superior separation capabilities. Porous nanofillers entice increased attention over nonporous counterparts due to their inherent CO2 uptake capacities and secondary transport pathways when added to polymer matrices. Infinite possibilities of tuning the porous architecture of these nanofillers also facilitate simultaneous enhancement of permeability, selectivity and stability features of the membrane conveniently heading in the direction towards industrial realization. This review focuses on presenting a complete synopsis of inherent capacities of several porous nanofillers, like metal organic frameworks (MOFs), Zeolites, and porous organic frameworks (POFs) and the effects on their addition to polymeric membranes. Gas permeation performances of select hybrids with these three-dimensional (3D) fillers and porous nanosheets have been summarized and discussed with respect to each type. Consequently, the benefits and shortcomings of each class of materials have been outlined and future research directions concerning the hybrids with 3D fillers have been suggested. Full article
(This article belongs to the Special Issue Mixed Matrix Membranes)
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