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Membranes
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Advancements of 2D Materials-Based Membranes
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Advancements of 2D Materials-Based Membranes

A special issue of Membranes (ISSN 2077-0375). This special issue belongs to the section "Inorganic Membranes".

Deadline for manuscript submissions: closed (30 July 2021) | Viewed by 26035

Special Issue Editor

Dr. Khaled A Mahmoud

E-Mail Website
Guest Editor
1. Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, P.O. Box 34110, Doha, Qatar
2. Center for Advanced Materials, Qatar University, Doha, Qatar
Interests: sustainable water treatment; environmental monitoring and remediation; membrane separation; antimicrobial nanomaterials; biocides nanocatalysis; energy storage; enhanced oil recovery applications; Specialized in 2D- carbon nanomaterials including MXene, graphenes, cellulose nanocrystals, and metal oxides

Special Issue Information

Dear Colleagues,

Two-dimensional (2D) materials such as graphenes, MXenes, MoS2, 2D covalent‐organic frameworks, and metal–organic frameworks are rapidly emerging in the development of membranes with high selectivity and permeability. Characteristic properties of 2D materials including high conductivity, hydrophilicity, rational tunability and precise control of interlayer spacing and/or nanochannles enable 2D materials-based membranes to achieve highly selective and precise separations. 2D materials sieving mechanism of target molecules is mainly governed by size exclusion through the ultrathin stacked architecture of 2D materials-based membranes and in some cases (such as in MXenes) interaction between the transported molecules and the charged layers. In recent years, several theoretical and experimental efforts were devoted to advance the rational design of predefined interlayer channels, membrane nanopores, and reasonable functionalization to overcome the tradeoff between selectivity and permeability of 2D nanomaterial‐based membranes.

This Special Issue is focusing on the recent advancements of the various 2D materials-based membranes. It covers all aspects associated with the synthesis and modifications of 2D materials, different fabrication methods of 2D materials based membranes, their separation mechanisms, and applications in various membrane-based processes, including desalination, wastewater treatment, gas separation, solvent purification, and oil/water separation.

Dr. Khaled A Mahmoud
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 2700 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

  • 2D materials
  • membranes
  • graphenes
  • MXenes
  • MoS2
  • metal–organic frameworks
  • molecular sieving
  • desalination
  • wastewater treatment

Published Papers (8 papers)

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Editorial

Jump to: Research, Review

3 pages, 185 KiB  
Editorial
Advancements of 2D Materials-Based Membranes
by Zakarya Othman and Khaled A. Mahmoud
Membranes 2022, 12(1), 52; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes12010052 - 31 Dec 2021
Cited by 1 | Viewed by 1420
Abstract
Our environment desperately needs creative solutions to limit the effect of industrialization’s fast rise and, consequently, to remediate vast amounts of harmful by-products and toxic exhausts [...] Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)

Research

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16 pages, 3055 KiB  
Article
MXene (Ti3C2Tx)/Cellulose Acetate Mixed-Matrix Membrane Enhances Fouling Resistance and Rejection in the Crossflow Filtration Process
by Reem S. Azam, Dema A. Almasri, Radwan Alfahel, Alaa H. Hawari, Mohammad K. Hassan, Ahmed A. Elzatahry and Khaled A. Mahmoud
Membranes 2022, 12(4), 406; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes12040406 - 06 Apr 2022
Cited by 8 | Viewed by 2234
Abstract
Obstacles in the membrane-based separation field are mainly related to membrane fouling. This study involved the synthesis and utilization of covalently crosslinked MXene/cellulose acetate mixed matrix membranes with MXene at different concentrations (CCAM-0% to CCAM-12%) for water purification applications. The membranes’ water flux, [...] Read more.
Obstacles in the membrane-based separation field are mainly related to membrane fouling. This study involved the synthesis and utilization of covalently crosslinked MXene/cellulose acetate mixed matrix membranes with MXene at different concentrations (CCAM-0% to CCAM-12%) for water purification applications. The membranes’ water flux, dye, and protein rejection performances were compared using dead-end (DE) and crossflow (CF) filtration. The fabricated membranes, especially CCAM-10%, exhibited high hydrophilicity, good surface roughness, significantly high water flux, high water uptake, and high porosity. A significantly higher flux was observed in CF filtration relative to DE filtration. Moreover, in CF filtration, the CCAM-10% membrane exhibited 96.60% and 99.49% rejection of methyl green (MG) and bovine serum albumin (BSA), respectively, while maintaining a flux recovery ratio of 67.30% and an irreversible fouling ratio at (Rir) of 32.70, indicating good antifouling performance. Hence, this study suggests that covalent modification of cellulose acetate membranes with MXene significantly improves the performance and fouling resistance of membranes for water filtration in CF mode relative to DE mode. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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12 pages, 4691 KiB  
Article
First-Principles Density Functional Theory Calculations of Bilayer Membranes Heterostructures of Ti3C2T2 (MXene)/Graphene and AgNPs
by Golibjon. R. Berdiyorov, Mohamed E. Madjet and Khaled. A. Mahmoud
Membranes 2021, 11(7), 543; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes11070543 - 16 Jul 2021
Cited by 10 | Viewed by 3962
Abstract
The properties of two-dimensional (2D) layered membrane systems can be medullated by the stacking arrangement and the heterostructure composition of the membrane. This largely affects the performance and stability of such membranes. Here, we have used first-principle density functional theory calculations to conduct [...] Read more.
The properties of two-dimensional (2D) layered membrane systems can be medullated by the stacking arrangement and the heterostructure composition of the membrane. This largely affects the performance and stability of such membranes. Here, we have used first-principle density functional theory calculations to conduct a comparative study of two heterostructural bilayer systems of the 2D-MXene (Ti3C2T2, T = F, O, and OH) sheets with graphene and silver nanoparticles (AgNPs). For all considered surface terminations, the binding energy of the MXene/graphene and MXene/AgNPs bilayers increases as compared with graphene/graphene and MXene/MXene bilayer structures. Such strong interlayer interactions are due to profound variations of electrostatic potential across the layers. Larger interlayer binding energies in MXene/graphene systems were obtained even in the presence of water molecules, indicating enhanced stability of such a hybrid system against delamination. We also studied the structural properties of Ti3C2X2 MXene (X = F, O and OH) decorated with silver nanoclusters Agn (n ≤ 6). We found that regardless of surface functionalization, Ag nanoclusters were strongly adsorbed on the surface of MXene. In addition, Ag nanoparticles enhanced the binding energy between MXene layers. These findings can be useful in enhancing the structural properties of MXene membranes for water purification applications. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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16 pages, 6324 KiB  
Article
Graphene Oxide Membranes for High Salinity, Produced Water Separation by Pervaporation
by Khalfan Almarzooqi, Mursal Ashrafi, Theeran Kanthan, Ali Elkamel and Michael A. Pope
Membranes 2021, 11(7), 475; https://doi.org/10.3390/membranes11070475 - 26 Jun 2021
Cited by 13 | Viewed by 2827
Abstract
Oil and gas industries produce a huge amount of wastewater known as produced water which contains diverse contaminants including salts, dissolved organics, dispersed oils, and solids making separation and purification challenging. The chemical and thermal stability of graphene oxide (GO) membranes make them [...] Read more.
Oil and gas industries produce a huge amount of wastewater known as produced water which contains diverse contaminants including salts, dissolved organics, dispersed oils, and solids making separation and purification challenging. The chemical and thermal stability of graphene oxide (GO) membranes make them promising for use in membrane pervaporation, which may provide a more economical route to purifying this water for disposal or re-use compared to other membrane-based separation techniques. In this study, we investigate the performance and stability of GO membranes cast onto polyethersulfone (PES) supports in the separation of simulated produced water containing high salinity brackish water (30 g/L NaCl) contaminated with phenol, cresol, naphthenic acid, and an oil-in-water emulsion. The GO/PES membranes achieve water flux as high as 47.8 L m−2 h−1 for NaCl solutions for membranes operated at 60 °C, while being able to reject 99.9% of the salt and upwards of 56% of the soluble organic components. The flux for membranes tested in pure water, salt, and simulated produced water was found to decrease over 72 h of testing but only to 50–60% of the initial flux in the worst-case scenario. This drop was concurrent with an increase in contact angle and C/O ratio indicating that the GO may become partially reduced during the separation process. Additionally, a closer look at the membrane crosslinker (Zn2+) was investigated and found to hydrolyze over time to Zn(OH)2 with much of it being washed away during the long-term pervaporation. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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11 pages, 3159 KiB  
Article
Reduced Graphene Oxide-Based Foam as an Endocrine Disruptor Adsorbent in Aqueous Solutions
by Jeanne N’Diaye, Sujittra Poorahong, Ons Hmam, Gastón Contreras Jiménez, Ricardo Izquierdo and Mohamed Siaj
Membranes 2020, 10(11), 340; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes10110340 - 13 Nov 2020
Cited by 8 | Viewed by 2753
Abstract
A stable and magnetic graphene oxide (GO) foam–polyethyleneimine–iron nanoparticle (GO–PEI–FeNPs) composite has been fabricated for removal of endocrine disruptors—bisphenol A, progesterone and norethisterone—from aqueous solution. The foam with porous and hierarchical structures was synthesized by reduction of graphene oxide layers coupled with co-precipitation [...] Read more.
A stable and magnetic graphene oxide (GO) foam–polyethyleneimine–iron nanoparticle (GO–PEI–FeNPs) composite has been fabricated for removal of endocrine disruptors—bisphenol A, progesterone and norethisterone—from aqueous solution. The foam with porous and hierarchical structures was synthesized by reduction of graphene oxide layers coupled with co-precipitation of iron under a hydrothermal system using polyethyleneimine as a cross linker. The presence of magnetic iron nanoparticles facilitates the separation process after decontamination. The foam was fully characterized by surface and structural scanning electron microscopy, Fourier transform infrared spectroscopy, Raman spectroscopy and X-ray photoelectron spectroscopy. The foam exhibits a high adsorption capacity, and the maximum adsorption percentages are 68%, 49% and 80% for bisphenol A, progesterone and norethisterone, respectively. The adsorption process of bisphenol A is explained according to the Langmuir model, whereas the Freundlich model was used for progesterone and norethisterone adsorption. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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11 pages, 2256 KiB  
Article
Graphene Oxide Membrane Immobilized Aptamer as a Highly Selective Hormone Removal
by Siham Chergui, Khaled Rhili, Sujittra Poorahong and Mohamed Siaj
Membranes 2020, 10(9), 229; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes10090229 - 12 Sep 2020
Cited by 8 | Viewed by 3063
Abstract
Three-dimensional (3D) reduced graphene oxide (rGO) modified by polyethyleneimine (PEI) was prepared and functionalized by fluorophore-labeled dexamethasone-aptamer (Flu-DEX-apt) via π–π stacking interaction. The rGO/PEI/Flu-DEX-apt was used as a selective membrane for dexamethasone hormone removal from water. The prepared rGO/PEI/Flu-DEX-apt membranes were stable, insoluble, [...] Read more.
Three-dimensional (3D) reduced graphene oxide (rGO) modified by polyethyleneimine (PEI) was prepared and functionalized by fluorophore-labeled dexamethasone-aptamer (Flu-DEX-apt) via π–π stacking interaction. The rGO/PEI/Flu-DEX-apt was used as a selective membrane for dexamethasone hormone removal from water. The prepared rGO/PEI/Flu-DEX-apt membranes were stable, insoluble, and easily removable from liquid media. The membrane was characterized by Raman spectroscopy, scanning electron spectroscopy, and FTIR spectroscopy. The rGO/PEI/Flu-DEX-apt membrane showed high sensitivity and specificity toward the dexamethasone hormone in the presence of other steroid hormone analogs, such as progesterone, estrone, estradiol, and 19-norethindrone. The fluorescence and UV–visible spectroscopy were used to confirm the membranes performance and the quantification of hormones removal. The resulting data clearly show that the graphene oxide concentration influence the aptamers and analytes interaction (π–π stacking interaction). It was found that by varying the graphene oxide concentration yields to different porosities of rGO/PEI/Flu-DEX-apt membranes affects the adsorption recovery rate, as well as the specificity and selectivity toward the dexamethasone hormone. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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Review

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17 pages, 7345 KiB  
Review
Recent Developments in Nanoporous Graphene Membranes for Organic Solvent Nanofiltration: A Short Review
by Yoon-Tae Nam, Jun-Hyeok Kang, Jae-Dong Jang, Jun-Hyuk Bae, Hee-Tae Jung and Dae-Woo Kim
Membranes 2021, 11(10), 793; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes11100793 - 18 Oct 2021
Cited by 9 | Viewed by 3922
Abstract
Graphene-based membranes are promising candidates for efficient organic solvent nanofiltration (OSN) processes because of their unique structural characteristics, such as mechanical/chemical stability and precise molecular sieving. Recently, to improve organic solvent permeance and selectivity, nanopores have been fabricated on graphene planes via chemical [...] Read more.
Graphene-based membranes are promising candidates for efficient organic solvent nanofiltration (OSN) processes because of their unique structural characteristics, such as mechanical/chemical stability and precise molecular sieving. Recently, to improve organic solvent permeance and selectivity, nanopores have been fabricated on graphene planes via chemical and physical methods. The nanopores serve as an additional channel for facilitating ultrafast solvent permeation while filtering organic molecules by size exclusion. This review summarizes the recent developments in nanoporous graphene (NG)-based membranes for OSN applications. The membranes are categorized depending on the membrane structure: single-layer NG, multilayer NG, and graphene-based composite membranes hybridized with other porous materials. Techniques for nanopore generation on graphene, as well as the challenges faced and the perspectives required for the commercialization of NG membranes, are also discussed. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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22 pages, 4011 KiB  
Review
Advances in the Synthesis and Application of Anti-Fouling Membranes Using Two-Dimensional Nanomaterials
by Asif Shahzad, Jae-Min Oh, Mudassar Azam, Jibran Iqbal, Sabir Hussain, Waheed Miran and Kashif Rasool
Membranes 2021, 11(8), 605; https://0-doi-org.brum.beds.ac.uk/10.3390/membranes11080605 - 09 Aug 2021
Cited by 11 | Viewed by 4521
Abstract
This article provides a comprehensive review of the recent progress in the application of advanced two-dimensional nanomaterials (2DNMs) in membranes fabrication and application for water purification. The membranes fouling, its types, and anti-fouling mechanisms of different 2DNMs containing membrane systems are also discussed. [...] Read more.
This article provides a comprehensive review of the recent progress in the application of advanced two-dimensional nanomaterials (2DNMs) in membranes fabrication and application for water purification. The membranes fouling, its types, and anti-fouling mechanisms of different 2DNMs containing membrane systems are also discussed. The developments in membrane synthesis and modification using 2DNMs, especially graphene and graphene family materials, carbon nanotubes (CNTs), MXenes, and others are critically reviewed. Further, the application potential of next-generation 2DNMs-based membranes in water/wastewater treatment systems is surveyed. Finally, the current problems and future opportunities of applying 2DNMs for anti-fouling membranes are also debated. Full article
(This article belongs to the Special Issue Advancements of 2D Materials-Based Membranes)
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