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Membranes
Volume 10
Issue 4
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Membranes, Volume 10, Issue 4 (April 2020) – 24 articles

Cover Story (view full-size image): We prepared and characterized mixed-matrix membranes based on amorphous PPO and particles of the molecular sieve ZIF-8. The inclusion of ZIF-8 with loadings as high as 45 wt % led to a remarkable, up to eight-fold, increase in gas permeability and to a significant decrease in the activation energy of diffusion and permeation. The ideal He/CO2 selectivity also increased, albeit to a lower extent, reaching a maximum at a filler loading of 35 wt %. The additive behavior observed in density measurements and the morphological analysis of the composite films indicate good adhesion between the two phases. The use of commercial materials enables the possibility of scaling-up the technology, and the results encourage applications at high temperatures. View this paper
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10 pages, 2950 KiB  
Article
Optimization of Air Backwash Frequency during the Ultrafiltration of Seawater
by Clemence Cordier, Tarik Eljaddi, Nadjim Ibouroihim, Christophe Stavrakakis, Patrick Sauvade, Franz Coelho and Philippe Moulin
Membranes 2020, 10(4), 78; https://doi.org/10.3390/membranes10040078 - 22 Apr 2020
Cited by 8 | Viewed by 3200
Abstract
The main objective of this paper is to study the effect of new air backwash on dead-end ultrafiltration of seawater with a pilot at semi-industrial scale (20 m3/day). To control membrane fouling, two different backwashes were used to clean the membrane: [...] Read more.
The main objective of this paper is to study the effect of new air backwash on dead-end ultrafiltration of seawater with a pilot at semi-industrial scale (20 m3/day). To control membrane fouling, two different backwashes were used to clean the membrane: classical backwash (CB) and new air backwash (AB) that consists of injecting air into the membrane module before a classical backwash. To evaluate the efficiency of AB and CB, a resistance in series model was used to calculate each resistance: membrane (Rm), reversible (Rrev) and irreversible (Rirr). The variation of the seawater quality was considered by integrating the turbidity variation versus time. The results indicate clearly that AB was more performant than CB and frequency of AB/CB cycles was important to control membrane fouling. In this study, frequencies of 1/5 and 1/3 appear more efficient than 1/7 and 1/9. In addition, the operation conditions (flux and time of filtration) had an important role in maintaining membrane performance—whatever the variation of the seawater quality. Full article
(This article belongs to the Special Issue Integrated Membrane Systems and Processes)
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22 pages, 5956 KiB  
Article
Experimental Investigation of the Effect of Implanting TiO2-NPs on PVC for Long-Term UF Membrane Performance to Treat Refinery Wastewater
by Faris H. Al-Ani, Qusay F. Alsalhy, Rawia Subhi Raheem, Khalid T. Rashid and Alberto Figoli
Membranes 2020, 10(4), 77; https://doi.org/10.3390/membranes10040077 - 21 Apr 2020
Cited by 59 | Viewed by 4028
Abstract
This study investigated the impact of implanting TiO2-NPs within a membrane to minimize the influence of long-term operation on the membrane characteristics. Four poly vinyle chloride-titanium oxide (PVC-TiO2-NPs) membranes were prepared to create an ultrafiltration membrane (UF) that would [...] Read more.
This study investigated the impact of implanting TiO2-NPs within a membrane to minimize the influence of long-term operation on the membrane characteristics. Four poly vinyle chloride-titanium oxide (PVC-TiO2-NPs) membranes were prepared to create an ultrafiltration membrane (UF) that would effectively treat actual refinery wastewater. The hypothesis of this work was that TiO2-NPs would function as a hydrophilic modification of the PVC membrane and excellent self-cleaning material, which in turn would greatly extend the membrane’s lifetime. The membranes were characterized via Fourier transforms infrared spectroscopy (FTIR), X-ray diffraction (XRD), energy dispersive X-ray (EDX), atomic force microscope (AFM), and scanning electron microscope (SEM). The removal efficiency of turbidity, total suspended solid (TSS), oil and grease, heavy metals and chemical oxygen demand (COD) were investigated. Contact angle (CA) reduced by 12.7% and 27.5% on the top and bottom surfaces, respectively. The PVC membrane with TiO2-NPs had larger mean pore size on its surface and more holes with larger size inside the membrane structure. The addition of TiO2-NPs could remarkably enhance the antifouling property of the PVC membrane. The pure water permeability (PWP) of the membrane was enhanced by 95.3% with an increase of TiO2 to 1.5 gm/100gm. The PWP after backwashing was reduced from 22.3% for PVC to 10.1% with 1.5 gm TiO2-NPs. The long-term performance was improved from five days for PVC to 23 d with an increase in TiO2-NPs to 1.5 gm. The improvements of PVC-TiO2-NPs long-term were related to the enhancement of the hydrophilic character of the membrane and increase tensile strength due to the reinforcement effect of TiO2-NPs. These results clearly identify the impact of the TiO2-NPs content on the long-term PVC/TiO2-NPs performance and confirm our hypothesis that it is possible to use TiO2-NPs to effectively enhance the lifetime of membranes during their long-term operation. Full article
(This article belongs to the Special Issue Membrane Preparation and Characterisation and Their Application in Environmental Field (Volume II))
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13 pages, 7438 KiB  
Article
The Effect of Emulsifiers on the Emulsion Stability and Extraction Efficiency of Cr(VI) Using Emulsion Liquid Membranes (ELMs) Formulated with a Green Solvent
by Katia Anarakdim, Gemma Gutiérrez, Ángel Cambiella, Ounissa Senhadji-Kebiche and María Matos
Membranes 2020, 10(4), 76; https://doi.org/10.3390/membranes10040076 - 21 Apr 2020
Cited by 27 | Viewed by 6040
Abstract
The stability of emulsion liquid membranes (ELMs) and their ability to extract Cr(VI) were investigated. The objective of this study is to compare different ELM formulations using combinations of two hydrophilic (Tween 20 and Tween 80) and two lipophilic (polyglycerol polyricinoleate (PGPR) and [...] Read more.
The stability of emulsion liquid membranes (ELMs) and their ability to extract Cr(VI) were investigated. The objective of this study is to compare different ELM formulations using combinations of two hydrophilic (Tween 20 and Tween 80) and two lipophilic (polyglycerol polyricinoleate (PGPR) and Span 80) emulsifiers. TOPO (tri-n-octylphosphine oxide) as a carrier and a green solvent (sunflower oil) were used to provide high extraction efficiency of Cr(VI). All these double emulsions were characterized in droplet size distribution, zeta potential, visual inspection with a microscope, and stability. The best formulation was obtained with PGPR as the inner stabilizer and Tween 80 as the outer stabilizer, leading to Cr(VI) ion removal efficiency of up to 96%. Full article
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13 pages, 2118 KiB  
Article
Enhanced O2/N2 Separation of Mixed-Matrix Membrane Filled with Pluronic-Compatibilized Cobalt Phthalocyanine Particles
by S. A. S. C. Samarasinghe, Chong Yang Chuah, H. Enis Karahan, G. S. M. D. P. Sethunga and Tae-Hyun Bae
Membranes 2020, 10(4), 75; https://doi.org/10.3390/membranes10040075 - 18 Apr 2020
Cited by 23 | Viewed by 5785
Abstract
Membrane-based air separation (O2/N2) is of great importance owing to its energy efficiency as compared to conventional processes. Currently, dense polymeric membranes serve as the main pillar of industrial processes used for the generation of O2- and [...] Read more.
Membrane-based air separation (O2/N2) is of great importance owing to its energy efficiency as compared to conventional processes. Currently, dense polymeric membranes serve as the main pillar of industrial processes used for the generation of O2- and N2-enriched gas. However, conventional polymeric membranes often fail to meet the selectivity needs owing to the similarity in the effective diameters of O2 and N2 gases. Meanwhile, mixed-matrix membranes (MMMs) are convenient to produce high-performance membranes while keeping the advantages of polymeric materials. Here, we propose a novel MMM for O2/N2 separation, which is composed of Matrimid® 5218 (Matrimid) as the matrix, cobalt(II) phthalocyanine microparticles (CoPCMPs) as the filler, and Pluronic® F-127 (Pluronic) as the compatibilizer. By the incorporation of CoPCMPs to Matrimid, without Pluronic, interfacial defects were formed. Pluronic-treated CoPCMPs, on the other hand, enhanced O2 permeability and O2/N2 selectivity by 64% and 34%, respectively. We explain the enhancement achieved with the increase of both O2 diffusivity and O2/N2 solubility selectivity. Full article
(This article belongs to the Special Issue Membranes for Gas Separation)
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17 pages, 4494 KiB  
Article
Leveraging Nanocrystal HKUST-1 in Mixed-Matrix Membranes for Ethylene/Ethane Separation
by Chong Yang Chuah, S.A.S.C. Samarasinghe, Wen Li, Kunli Goh and Tae-Hyun Bae
Membranes 2020, 10(4), 74; https://doi.org/10.3390/membranes10040074 - 16 Apr 2020
Cited by 39 | Viewed by 6256
Abstract
The energy-intensive ethylene/ethane separation process is a key challenge to the petrochemical industry. HKUST-1, a metal–organic framework (MOF) which possesses high accessible surface area and porosity, is utilized in mixed-matrix membrane fabrication to investigate its potential for improving the performance for C2 [...] Read more.
The energy-intensive ethylene/ethane separation process is a key challenge to the petrochemical industry. HKUST-1, a metal–organic framework (MOF) which possesses high accessible surface area and porosity, is utilized in mixed-matrix membrane fabrication to investigate its potential for improving the performance for C2H4/C2H6 separation. Prior to membrane fabrication and gas permeation analysis, nanocrystal HKUST-1 was first synthesized. This step is critical in order to ensure that defect-free mixed-matrix membranes can be formed. Then, polyimide-based polymers, ODPA-TMPDA and 6FDA-TMPDA, were chosen as the matrices. Our findings revealed that 20 wt% loading of HKUST-1 was capable of improving C2H4 permeability (155% for ODPA-TMPDA and 69% for 6FDA-TMPDA) without excessively sacrificing the C2H4/C2H6 selectivity. The C2H4 and C2H6 diffusivity, as well as solubility, were also improved substantially as compared to the pure polymeric membranes. Overall, our results edge near the upper bound, confirming the effectiveness of leveraging nanocrystal HKUST-1 filler for performance enhancements in mixed-matrix membranes for C2H4/C2H6 separation. Full article
(This article belongs to the Special Issue Membranes for Gas Separation)
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33 pages, 2983 KiB  
Article
Comparison and Combination of Organic Solvent Nanofiltration and Adsorption Processes: A Mathematical Approach for Mitigation of Active Pharmaceutical Ingredient Losses during Genotoxin Removal
by Flávio Ferreira, Leonor Resina, Teresa Esteves and Frederico Castelo Ferreira
Membranes 2020, 10(4), 73; https://doi.org/10.3390/membranes10040073 - 16 Apr 2020
Cited by 8 | Viewed by 4417
Abstract
Active pharmaceutical ingredients (API) are synthesized using highly reactive reagents, catalysts, and solvents. Some of those persist as impurities in the final product and are genotoxic or carcinogenic. The conventional processes used for API purification and isolation are able to achieve the limits [...] Read more.
Active pharmaceutical ingredients (API) are synthesized using highly reactive reagents, catalysts, and solvents. Some of those persist as impurities in the final product and are genotoxic or carcinogenic. The conventional processes used for API purification and isolation are able to achieve the limits imposed by regulatory agencies, but at the expense of significant API losses. Here we report the development of a model to aid in the decision of which dedicated purification process, membrane or adsorption, is most suitable for removal of genotoxic impurities (GTIs), according with a small set of key intrinsic parameters. A hybrid process was developed, combining these two unit operations, to be applied when the use of OSN or adsorption alone result on non-acceptable API losses. Membrane solute rejection and solvent flux was used as parameter for OSN. In the case of adsorption, two isotherm models, Langmuir and Freundlich, were considered. The effect of the recirculation stream and amount of adsorber used on the hybrid process was investigated. Case studies were experimentally validated, confirming that combining the two unit operations can reduce API loss from 24.76% in OSN to 9.76% in a hybrid process. Economic and environmental analyses were performed. Full article
(This article belongs to the Special Issue Process of Membrane Separation: Comparison with Competing Traditional Processes)
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14 pages, 3686 KiB  
Article
Modeling and Simulation of the Simultaneous Absorption/Stripping of CO2 with Potassium Glycinate Solution in Membrane Contactor
by Nayef Ghasem
Membranes 2020, 10(4), 72; https://doi.org/10.3390/membranes10040072 - 16 Apr 2020
Cited by 11 | Viewed by 3837
Abstract
Global warming is an environmental problem caused mainly by one of the most serious greenhouse gas, CO2 emissions. Subsequently, the capture of CO2 from flue gas and natural gas is essential. Aqueous potassium glycinate (PG) is a promising novelty solvent used [...] Read more.
Global warming is an environmental problem caused mainly by one of the most serious greenhouse gas, CO2 emissions. Subsequently, the capture of CO2 from flue gas and natural gas is essential. Aqueous potassium glycinate (PG) is a promising novelty solvent used in the CO2 capture compared to traditional solvents; simultaneous solvent regeneration is associated with the absorption step. In present work, a 2D mathematical model where radial and axial diffusion are considered is developed for the simultaneous absorption/stripping process. The model describes the CO2/PG absorption/stripping process in a solvent–gas membrane absorption process. Regeneration data of rich potassium glycinate solvent using a varied range of acid gas loading (mol CO2 per mol PG) were used to predict the reversible reaction rate constant. A comparison of simulation results and experimental data validated the accuracy of the model predictions. The stripping reaction rate constant of rich potassium glycinate was determined experimentally and found to be a function of temperature and PG concentration. Model predictions were in good agreement with the experimental data. The results reveal that the percent removal of CO2 is directly proportional to CO2 loading and solvent stripping temperature. Full article
(This article belongs to the Special Issue Membranes: 10th Anniversary)
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25 pages, 7729 KiB  
Article
Structural, Morphological, Electrical and Electrochemical Properties of PVA: CS-Based Proton-Conducting Polymer Blend Electrolytes
by Ayub Shahab Marf, Ranjdar M. Abdullah and Shujahadeen B. Aziz
Membranes 2020, 10(4), 71; https://doi.org/10.3390/membranes10040071 - 15 Apr 2020
Cited by 69 | Viewed by 4258
Abstract
Polymer blend electrolytes based on poly(vinyl alcohol):chitosan (PVA:CS) incorporated with various quantities of ammonium iodide were prepared and characterized using a range of electrochemical, structural and microscopic techniques. In the structural analysis, X-ray diffraction (XRD) was used to confirm the buildup of the [...] Read more.
Polymer blend electrolytes based on poly(vinyl alcohol):chitosan (PVA:CS) incorporated with various quantities of ammonium iodide were prepared and characterized using a range of electrochemical, structural and microscopic techniques. In the structural analysis, X-ray diffraction (XRD) was used to confirm the buildup of the amorphous phase. To reveal the effect of dopant addition on structural changes, field-emission scanning electron microscope (FESEM) was used. The protrusions of salt aggregates with large quantity were seen at the surface of the formed films at 50 wt.% of the added salt. The nature of the relationship between conductivity and dielectric properties was shown using electrochemical impedance spectroscopy (EIS). The EIS spectra were fitted with electrical equivalent circuits (EECs). It was observed that both dielectric constant and dielectric loss were high in the low-frequency region. For all samples, loss tangent and electric modulus plots were analyzed to become familiar with the relaxation behavior. Linear sweep voltammetry (LSV) and transference number measurement (TNM) were recorded. A relatively high cut-off potential for the polymer electrolyte was obtained at 1.33 V and both values of the transference number for ion (tion) and electronic (telec) showed the ion dominant as charge carrier species. The TNM and LSV measurements indicate the suitability of the samples for energy storage application if their conductivity can be more enhanced. Full article
(This article belongs to the Special Issue Ionic Conductive Membranes for Fuel Cells)
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16 pages, 5446 KiB  
Article
Mesoporous Silica Membranes Silylated by Fluorinated and Non-Fluorinated Alkylsilanes for the Separation of Methyl Tert-Butyl Ether from Water
by Zhaojia Wang, Liwei Hao, Feihua Yang and Qi Wei
Membranes 2020, 10(4), 70; https://doi.org/10.3390/membranes10040070 - 15 Apr 2020
Cited by 15 | Viewed by 4294
Abstract
It is of great significance to separate hazardous methyl tert-butyl ether (MTBE) from water in terms of environmental protection and human health. In the present work, α-Al2O3-suppotred silica membranes were prepared by the sol-gel and dip-coating technique. Two fluorinated [...] Read more.
It is of great significance to separate hazardous methyl tert-butyl ether (MTBE) from water in terms of environmental protection and human health. In the present work, α-Al2O3-suppotred silica membranes were prepared by the sol-gel and dip-coating technique. Two fluorinated alkylsilanes (1H,1H,2H,2H-perfluorooctyltriethoxysilane (PFOTES) and trifluoropropyltriethoxysilane (TFPTES)) and two non-fluorinated alkylsilanes (octyltriethoxysilane (OTES) and propyltriethoxysilane (PTES)) were adopted to silylate the silica membrane by the post-grafting method which is used for the separation of MTBE from water by pervaporation. The results show that silylation enhances the hydrophobicity of silica membranes. The silylated silica membranes are selective towards MTBE, and the MTBE/water separation factor varies with grafting agents in the order: PFOTES > TFPTES > OTES > PTES. Membranes silylated with fluorinated carbon chains seem to be more selective towards MTBE than those with non-fluorinated carbon chains. The total flux is proportional to the pore volume of silica membranes, which depends on grafting agents in the order: PTES > PFOTES > OTES > TFPTES. Considering both total flux and selectivity, the PFOTES-SiO2 membrane is most effective in separation, with a MTBE/water separation factor of 24.6 and a total flux of 0.35 kg m−2 h−1 under a MTBE concentration of 3.0% and a feed temperature of 30 °C. Full article
(This article belongs to the Special Issue Pervaporation, Vapour Permeation and Membrane Distillation: From Membrane Fabrication to Application)
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21 pages, 4808 KiB  
Article
Treatment of Cyanide-Free Wastewater from Brass Electrodeposition with EDTA by Electrodialysis: Evaluation of Underlimiting and Overlimiting Operations
by Kayo Santana Barros, Tatiana Scarazzato, Valentín Pérez-Herranz and Denise Crocce Romano Espinosa
Membranes 2020, 10(4), 69; https://doi.org/10.3390/membranes10040069 - 11 Apr 2020
Cited by 23 | Viewed by 4338
Abstract
Growing environmental concerns have led to the development of cleaner processes, such as the substitution of cyanide in electroplating industries and changes in the treatment of wastewaters. Hence, we evaluated the treatment of cyanide-free wastewater from the brass electroplating industry with EDTA as [...] Read more.
Growing environmental concerns have led to the development of cleaner processes, such as the substitution of cyanide in electroplating industries and changes in the treatment of wastewaters. Hence, we evaluated the treatment of cyanide-free wastewater from the brass electroplating industry with EDTA as a complexing agent by electrodialysis, aimed at recovering water and concentrated solutions for reuse. The electrodialysis tests were performed in underlimiting and overlimiting conditions. The results suggested that intense water dissociation occurred at the cathodic side of the commercial anion-exchange membrane (HDX) during the overlimiting test. Consequently, the pH reduction at this membrane may have led to the reaction of protons with complexes of EDTA-metals and insoluble species. This allowed the migration of free Cu2+ and Zn2+ to the cation-exchange membrane as a result of the intense electric field and electroconvection. These overlimiting phenomena accounted for the improvement of the percent extraction and percent concentration, since in the electrodialysis stack employed herein, the concentrate compartments of cationic and anionic species were connected to the same reservoir. Chronopotentiometric studies showed that electroconvective vortices minimized fouling/scaling at both membranes. The electrodialysis in the overlimiting condition seemed to be more advantageous due to water dissociation and electroconvection. Full article
(This article belongs to the Special Issue Electromembrane Processes: Emerging Applications, Materials and Process Configurations)
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17 pages, 4667 KiB  
Article
Particle Track and Trace during Membrane Filtration by Direct Observation with a High Speed Camera
by Mads Koustrup Jørgensen, Kristian Boe Eriksen and Morten Lykkegaard Christensen
Membranes 2020, 10(4), 68; https://doi.org/10.3390/membranes10040068 - 10 Apr 2020
Cited by 6 | Viewed by 3196
Abstract
A methodology was developed for direct observation and analysis of particle movements near a microfiltration membrane. A high speed camera (1196 frames per second) was mounted on a microscope to record a hollow fiber membrane in a filtration cell with a transparent wall. [...] Read more.
A methodology was developed for direct observation and analysis of particle movements near a microfiltration membrane. A high speed camera (1196 frames per second) was mounted on a microscope to record a hollow fiber membrane in a filtration cell with a transparent wall. Filtrations were conducted at varying pressure and crossflow velocities using synthetic core–shell particles (diameter 1.6 μm) of no and high negative surface charge. MATLAB scripts were developed to track the particle positions and calculate velocities of particle movements across and towards the membrane surface. Data showed that the velocity of particles along the membrane increases with distance from the membrane surface which correlates well with a fluid velocity profile obtained from CFD modelling. Particle track and trace was used to calculate the particle count profiles towards the membrane and document a higher concentration of particles near the membrane surface than in the bulk. Calculation of particle velocity towards and away from the membrane showed a region within 3–80 μm from the membrane surface with particle velocities higher than expected from the velocity of water through the membrane, thus the permeation drag underpredicts the actual velocity of particles towards the membrane. Near the membrane, particle velocities shift direction and move away. This is not described in classical filtration theory, but it has been speculated that this is an effect of particle rotation or due to membrane vibration or change in flow pattern close to the membrane. Full article
(This article belongs to the Special Issue Fouling and Cleaning in Membrane Processes, Volume II)
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23 pages, 2843 KiB  
Article
Cross-Flow Microfiltration of Glycerol Fermentation Broths with Citrobacter freundii
by Wirginia Tomczak and Marek Gryta
Membranes 2020, 10(4), 67; https://doi.org/10.3390/membranes10040067 - 8 Apr 2020
Cited by 15 | Viewed by 4419
Abstract
This paper reports the study of the cross-flow microfiltration (MF) of glycerol fermentation broths with Citrobacter freundii bacteria. A single channel tubular ceramic membrane with a nominal pore size of 0.14 µm was used. It has been demonstrated that the MF ceramic membrane [...] Read more.
This paper reports the study of the cross-flow microfiltration (MF) of glycerol fermentation broths with Citrobacter freundii bacteria. A single channel tubular ceramic membrane with a nominal pore size of 0.14 µm was used. It has been demonstrated that the MF ceramic membrane has been successfully applied to bacteria cell removal and to effectively eliminate colloidal particles from glycerol fermentation broths. However, due to fouling, the significant reduction of the MF performance has been demonstrated. In order to investigate the impact of transmembrane pressure (TMP) and feed flow rate (Q) on MF performance, 24 experiments have been performed. The highest steady state permeate flux (138.97 dm3/m2h) was achieved for 0.12 MPa and 1000 dm3/h. Fouling analysis has been studied based on the resistance-in series model. It has been found that the percentage of irreversible fouling resistance during the MF increases with increasing TMP and Q. The permeate flux regeneration has been achieved by membrane cleaning with 3 wt % NaOH and 3 wt % H3PO4 at 45 °C. The results of this study are expected to be useful in industrially employing the MF process as the first step of glycerol fermentation broth purification. Full article
(This article belongs to the Special Issue Membranes: 10th Anniversary)
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17 pages, 8781 KiB  
Article
Improved Performance of Polysulfone Ultrafiltration Membrane Using TCPP by Post-Modification Method
by Yuandong Jia, Shuangqing Sun, Shunshun Li, Zhikun Wang, Fushan Wen, Chunling Li, Hideto Matsuyama and Songqing Hu
Membranes 2020, 10(4), 66; https://doi.org/10.3390/membranes10040066 - 7 Apr 2020
Cited by 7 | Viewed by 5085
Abstract
Ultrafiltration (UF) membranes have found great application in sewage purification and desalination due to their high permeation flux and high rejection rate for contaminants under low-pressure conditions, but the flux and antifouling ability of UF membranes needs to be improved. Tetrakis (4-carboxyphenyl) porphyrin [...] Read more.
Ultrafiltration (UF) membranes have found great application in sewage purification and desalination due to their high permeation flux and high rejection rate for contaminants under low-pressure conditions, but the flux and antifouling ability of UF membranes needs to be improved. Tetrakis (4-carboxyphenyl) porphyrin (TCPP) has good hydrophilicity, and it is protonated under strongly acidic conditions and then forms strong hydrogen bonds with N, O and S, so that the TCPP would be well anchored in the membrane. In this work, NaHCO3 was used to dissolve TCPP and TMC (trimesoyl chloride) was used to produce a strong acid. Then, TCPP was modified in a membrane with a different rejection rate by a method similar to interfacial polymerization. Performance tests of TCPP/polysulfone (PSf) membranes show that for the membrane with a high BSA (bovine serum albumin) rejection, when the ratio of NaHCO3 to TCPP is 16:1 (wt.%), the pure water flux of membrane Z1 16:1 is increased by 34% (from 455 to 614 Lm−2h−1bar−1) while the membrane retention was maintained above 95%. As for the membrane with a low BSA rejection, when the ratio of NaHCO3 to TCPP was 32:1, the rejection of membrane B2 32:1 was found to increase from 81% to 96%. Although the flux of membrane B2 32:1 decreased, it remained at 638 Lm−2h−1bar−1, which is comparable to the reported polymer ultrafiltration membrane. The above dual results are thought to be attributed to the synergistic effect of protonated TCPP and NaHCO3, where the former increases membrane flux and the latter increases the membrane rejection rate. This work provides a way for the application of porphyrin and porphyrin framework materials in membrane separation. Full article
(This article belongs to the Section Polymeric Membranes)
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18 pages, 2272 KiB  
Review
A Review on Current Development of Membranes for Oil Removal from Wastewaters
by Brian Bolto, Jianhua Zhang, Xing Wu and Zongli Xie
Membranes 2020, 10(4), 65; https://doi.org/10.3390/membranes10040065 - 7 Apr 2020
Cited by 62 | Viewed by 6519
Abstract
The current situation with the problems associated with the removal of oil from wastewaters by membranes is being explored. Many types of membranes have been investigated—organic polymers, inorganic or ceramic species and hybrids of the two. Polymeric membranes can be designed to facilitate [...] Read more.
The current situation with the problems associated with the removal of oil from wastewaters by membranes is being explored. Many types of membranes have been investigated—organic polymers, inorganic or ceramic species and hybrids of the two. Polymeric membranes can be designed to facilitate the passage of oil, but the more successful approach is with hydrophilic types that encourage the passage of water. Ceramic membranes have an advantage here as they are less often irreversibly fouled and give a higher recovery of oil, with a lower flux decline. Furthermore, they can be cleaned up by a simple heating procedure. More attention should be given to understanding the mechanism of fouling so that operating conditions can be optimised to further reduce fouling and further decrease the flux decline, as well as assisting in the design of antifouling membranes. Another obstacle to ceramic membrane use is the high cost of manufacture. Cheaper starting materials such as clays have been surveyed. Full article
(This article belongs to the Special Issue Theoretical and Experimental Investigation of the Mass and Heat Transfers in Membrane Separation Processes)
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14 pages, 4342 KiB  
Article
Influence of Ozone Treatment on Ultrafiltration Performance and Nutrient Flow in a Membrane Based Nutrient Recovery Process from Anaerobic Digestate
by Tobias Gienau, Artjom Ehrmanntraut, Matthias Kraume and Sandra Rosenberger
Membranes 2020, 10(4), 64; https://doi.org/10.3390/membranes10040064 - 4 Apr 2020
Cited by 10 | Viewed by 4409
Abstract
Membrane filtration of biological suspensions is frequently limited by fouling. This mechanism is well understood for ultrafiltration of activated sludge in membrane bioreactors. A rather young application of ultrafiltration is the recovery of nutrients from anaerobic digestates, e.g., from agricultural biogas plants. A [...] Read more.
Membrane filtration of biological suspensions is frequently limited by fouling. This mechanism is well understood for ultrafiltration of activated sludge in membrane bioreactors. A rather young application of ultrafiltration is the recovery of nutrients from anaerobic digestates, e.g., from agricultural biogas plants. A process chain of solid/liquid separation, ultrafiltration, and reverse osmoses separates the digestate into different products: an organic N-P-fertilizer (solid digestate), a recirculate (UF retentate), a liquid N-K-fertilizer (RO retentate) and water. Despite the preceding particle removal, high crossflow velocities are required in the ultrafiltration step to overcome fouling. This leads to high operation costs of the ultrafiltration step and often limits the economical application of the complete process chain. In this study, under-stoichiometric ozone treatment of the ultrafiltration feed stream is investigated. Ozone treatment reduced the biopolymer concentration and apparent viscosity of different digestate centrates. Permeabilities of centrate treated with ozone were higher than without ozone treatment. In a laboratory test rig and in a pilot plant operated at the site of two full scale biogas plants, ultrafiltration flux could be improved by 50–80% by ozonation. Nutrient concentrations in the fertilizer products were not affected by ozone treatment. Full article
(This article belongs to the Special Issue Membrane Technologies for Nutrient Recovery)
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18 pages, 9695 KiB  
Article
Influence of the Natural Zeolite Particle Size Toward the Ammonia Adsorption Activity in Ceramic Hollow Fiber Membrane
by Mohd Ridhwan Adam, Mohd Hafiz Dzarfan Othman, Siti Hamimah Sheikh Abdul Kadir, Mohd Nazri Mohd Sokri, Zhong Sheng Tai, Yuji Iwamoto, Masaki Tanemura, Sawao Honda, Mohd Hafiz Puteh, Mukhlis A. Rahman and Juhana Jaafar
Membranes 2020, 10(4), 63; https://doi.org/10.3390/membranes10040063 - 4 Apr 2020
Cited by 21 | Viewed by 5906
Abstract
Natural zeolite is widely used in removing ammonia via adsorption process because of its superior ion-exchange properties. Ceramic particle size affects the adsorptivity of particles toward ammonia. In this study, hollow fiber ceramic membrane (HFCM) was fabricated from natural zeolite via phase inversion. [...] Read more.
Natural zeolite is widely used in removing ammonia via adsorption process because of its superior ion-exchange properties. Ceramic particle size affects the adsorptivity of particles toward ammonia. In this study, hollow fiber ceramic membrane (HFCM) was fabricated from natural zeolite via phase inversion. The effect of natural zeolite particle size toward the properties and performance of HFCM was evaluated. The results show that the HFCM with smaller particle sizes exhibited a more compact morphological structure with better mechanical strength. The adsorption performance of HFCM was significantly improved with smaller particle sizes because of longer residence time, as proven by the lower water permeability. A high adsorption performance of 96.67% was achieved for HFCM with the smallest particle size (36 μm). These findings provide a new perspective on the promising properties of the natural zeolite-derived HFCM for ammonia removal. Full article
(This article belongs to the Special Issue Membranes: 10th Anniversary)
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12 pages, 1719 KiB  
Article
Effect of Bridgehead Methyl Substituents on the Gas Permeability of Tröger’s-Base Derived Polymers of Intrinsic Microporosity
by Richard Malpass-Evans, Ian Rose, Alessio Fuoco, Paola Bernardo, Gabriele Clarizia, Neil B. McKeown, Johannes C. Jansen and Mariolino Carta
Membranes 2020, 10(4), 62; https://doi.org/10.3390/membranes10040062 - 3 Apr 2020
Cited by 21 | Viewed by 4606
Abstract
A detailed comparison of the gas permeability of four Polymers of Intrinsic Microporosity containing Tröger’s base (TB-PIMs) is reported. In particular, we present the results of a systematic study of the differences between four related polymers, highlighting the importance of the role of [...] Read more.
A detailed comparison of the gas permeability of four Polymers of Intrinsic Microporosity containing Tröger’s base (TB-PIMs) is reported. In particular, we present the results of a systematic study of the differences between four related polymers, highlighting the importance of the role of methyl groups positioned at the bridgehead of ethanoanthracene (EA) and triptycene (Trip) components. The PIMs show BET surface areas between 845–1028 m2 g−1 and complete solubility in chloroform, which allowed for the casting of robust films that provided excellent permselectivities for O2/N2, CO2/N2, CO2/CH4 and H2/CH4 gas pairs so that some data surpass the 2008 Robeson upper bounds. Their interesting gas transport properties were mostly ascribed to a combination of high permeability and very strong size-selectivity of the polymers. Time lag measurements and determination of the gas diffusion coefficient of all polymers revealed that physical ageing strongly increased the size-selectivity, making them suitable for the preparation of thin film composite membranes. Full article
(This article belongs to the Special Issue Membranes for Gas Separation)
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15 pages, 2031 KiB  
Article
Assessment of Layer-By-Layer Modified Nanofiltration Membrane Stability in Phosphoric Acid
by Kirsten Remmen, Barbara Müller, Joachim Köser, Matthias Wessling and Thomas Wintgens
Membranes 2020, 10(4), 61; https://doi.org/10.3390/membranes10040061 - 3 Apr 2020
Cited by 14 | Viewed by 3457
Abstract
Nanofiltration (NF) can enable P recovery from waste streams via retaining multivalent impurities from spent pickling acid. However, with the currently available membranes, an economically feasible process is impossible. Layer-by-layer modified NF membranes are a promising solution for the recovery of P from [...] Read more.
Nanofiltration (NF) can enable P recovery from waste streams via retaining multivalent impurities from spent pickling acid. However, with the currently available membranes, an economically feasible process is impossible. Layer-by-layer modified NF membranes are a promising solution for the recovery of P from acidic leachate. LbL membranes show a high level of versatility in terms of fine tuning for ion retention, which is necessary to achieve sufficient phosphorus yields. However, the stability of layer-by-layer modified membranes during phosphoric acid (H3PO4) filtration needs to be further investigated. In our study, we show that a polyethersulfone hollow fiber membrane modified with four or eight bi-layers was stable during immersing and filtering of a 15% H3PO4 solution. A sulfonated polyethersulfone (sPES)-based hollow fiber LbL membrane was only stable during filtration. Thus, we show the importance of applying real process conditions to evaluate membranes. Another important aspect is the influence of the high ionic strength of the feed solution on the membrane. We show that a high ionic strength led to a decrease in Mg retention, which could be increased to 85% by adjusting the process parameters. Full article
(This article belongs to the Special Issue Membrane Technologies for Nutrient Recovery)
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15 pages, 2158 KiB  
Article
N,N’-Bis(salicylidene)ethylenediamine (Salen) as an Active Compound for the Recovery of Ni(II), Cu(II), and Zn(II) Ions from Aqueous Solutions
by Katarzyna Witt, Daria Bożejewicz and Małgorzata A. Kaczorowska
Membranes 2020, 10(4), 60; https://doi.org/10.3390/membranes10040060 - 2 Apr 2020
Cited by 8 | Viewed by 4521
Abstract
In this paper, three main methods of metal ion separation, i.e., liquid–liquid extraction, transport across polymer inclusion membranes (PIMs), and sorption/desorption, are described. In all of them, N,N’-bis(salicylidene)ethylenediamine (salen) was used as an active compound, i.e., as an extractant or [...] Read more.
In this paper, three main methods of metal ion separation, i.e., liquid–liquid extraction, transport across polymer inclusion membranes (PIMs), and sorption/desorption, are described. In all of them, N,N’-bis(salicylidene)ethylenediamine (salen) was used as an active compound, i.e., as an extractant or as a carrier for the recovery of Ni(II), Cu(II), or Zn(II) ions from aqueous solutions. In each case, the recovery was performed on a model solution, which contained only a single metal ion. The obtained results were compared with the author’s previous results for the separation of metal ions using β-diketones, since both β-diketones and salen form the so-called Werner-type complexes. Electrospray ionization high-resolution mass spectrometry (ESI-HRMS) was also applied to confirm the ability of the carrier to form complexes with metal ions in a solution. Moreover, spectrophotometry was used to determine the stability constant of the obtained complexes. Full article
(This article belongs to the Special Issue Selected Papers from XIII Scientific Conference “Membranes and Membrane Processes in Environmental Protection” (MEMPEP 2021))
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18 pages, 4732 KiB  
Article
Structural Characterisation of Deposit Layer during Milk Protein Microfiltration by Means of In-Situ MRI and Compositional Analysis
by Roland Schopf, Nicolas Schork, Estelle Amling, Hermann Nirschl, Gisela Guthausen and Ulrich Kulozik
Membranes 2020, 10(4), 59; https://doi.org/10.3390/membranes10040059 - 31 Mar 2020
Cited by 10 | Viewed by 4031
Abstract
Milk protein fractionation by microfiltration membranes is an established but still growing field in dairy technology. Even under cross-flow conditions, this filtration process is impaired by the formation of a deposit by the retained protein fraction, mainly casein micelles. Due to deposition formation [...] Read more.
Milk protein fractionation by microfiltration membranes is an established but still growing field in dairy technology. Even under cross-flow conditions, this filtration process is impaired by the formation of a deposit by the retained protein fraction, mainly casein micelles. Due to deposition formation and consequently increased overall filtration resistance, the mass flow of the smaller whey protein fraction declines within the first few minutes of filtration. Currently, there are only a handful of analytical techniques available for the direct observation of deposit formation with opaque feed media and membranes. Here, we report on the ongoing development of a non-invasive and non-destructive method based on magnetic resonance imaging (MRI), and its application to characterise deposit layer formation during milk protein fractionation in ceramic hollow fibre membranes as a function of filtration pressure and temperature, temporally and spatially resolved. In addition, the chemical composition of the deposit was analysed by reversed phase high pressure liquid chromatography (RP-HPLC). We correlate the structural information gained by in-situ MRI with the protein amount and composition of the deposit layer obtained by RP-HPLC. We show that the combination of in-situ MRI and chemical analysis by RP-HPLC has the potential to allow for a better scientific understanding of the pressure and temperature dependence of deposit layer formation. Full article
(This article belongs to the Section Membrane Analysis and Characterization)
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19 pages, 7025 KiB  
Article
The Influence of Graphene Addition on the Properties of Composite rGO/PAN Membranes and Their Potential Application for Water Disinfection
by Beata Fryczkowska, Alicja Machnicka, Dorota Biniaś, Czesław Ślusarczyk and Janusz Fabia
Membranes 2020, 10(4), 58; https://doi.org/10.3390/membranes10040058 - 29 Mar 2020
Cited by 11 | Viewed by 3111
Abstract
The paper presents a method of obtaining composite polyacrylonitrile-based (PAN) membranes with the addition of reduced graphene oxide (rGO). The membranes were obtained using phase inversion method from a homogeneous rGO dispersion in a solution of PAN dissolved in N, N-dimethylformamide (DMF). The [...] Read more.
The paper presents a method of obtaining composite polyacrylonitrile-based (PAN) membranes with the addition of reduced graphene oxide (rGO). The membranes were obtained using phase inversion method from a homogeneous rGO dispersion in a solution of PAN dissolved in N, N-dimethylformamide (DMF). The impact of the amount of rGO addition to the PAN matrix on the physicochemical, structural, transport, and separation properties and on fouling resistance was studied. Composite membranes, due to the method of preparation used and the addition of rGO, are characterized by very good transport properties (~390 L/m2 h) and by a high degree of protein retention (85%). Reduced graphene oxide has biocidal properties, which, as we have shown, depend on the size of nanoparticles and the type of microorganism. rGO/PAN membranes, on the other hand, show biostatic properties against Gram-negative bacteria (Escherichia coli), Gram-positive bacteria (Staphylococcuc aureus) and fungi (Candida albicans). Thus, the obtained composite membranes can be potentially used in water disinfection. Full article
(This article belongs to the Special Issue Membranes for Water Disinfection)
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34 pages, 11392 KiB  
Article
Enhancing the Separation Performance of Glassy PPO with the Addition of a Molecular Sieve (ZIF-8): Gas Transport at Various Temperatures
by Francesco M. Benedetti, Maria Grazia De Angelis, Micaela Degli Esposti, Paola Fabbri, Alice Masili, Alessandro Orsini and Alberto Pettinau
Membranes 2020, 10(4), 56; https://doi.org/10.3390/membranes10040056 - 27 Mar 2020
Cited by 18 | Viewed by 5236
Abstract
In this study, we prepared and characterized composite films formed by amorphous poly(2,6-dimethyl-1,4-phenylene oxide) (PPO) and particles of the size-selective Zeolitic Imidazolate Framework 8 (ZIF-8). The aim was to increase the permselectivity properties of pure PPO using readily available materials to enable the [...] Read more.
In this study, we prepared and characterized composite films formed by amorphous poly(2,6-dimethyl-1,4-phenylene oxide) (PPO) and particles of the size-selective Zeolitic Imidazolate Framework 8 (ZIF-8). The aim was to increase the permselectivity properties of pure PPO using readily available materials to enable the possibility to scale-up the technology developed in this work. The preparation protocol established allowed robust membranes with filler loadings as high as 45 wt% to be obtained. The thermal, morphological, and structural properties of the membranes were analyzed via DSC, SEM, TGA, and densitometry. The gas permeability and diffusivity of He, CO2, CH4, and N2 were measured at 35, 50, and 65 °C. The inclusion of ZIF-8 led to a remarkable increase of the gas permeability for all gases, and to a significant decrease of the activation energy of diffusion and permeation. The permeability increased up to +800% at 45 wt% of filler, reaching values of 621 Barrer for He and 449 for CO2 at 35 °C. The ideal size selectivity of the PPO membrane also increased, albeit to a lower extent, and the maximum was reached at a filler loading of 35 wt% (1.5 for He/CO2, 18 for CO2/N2, 17 for CO2/CH4, 27 for He/N2, and 24 for He/CH4). The density of the composite materials followed an additive behavior based on the pure values of PPO and ZIF-8, which indicates good adhesion between the two phases. The permeability and He/CO2 selectivity increased with temperature, which indicates that applications at higher temperatures than those inspected should be encouraged. Full article
(This article belongs to the Special Issue Polymer Membranes for Gas Separation)
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18 pages, 4188 KiB  
Article
Influence of Spacer Design and Module Geometry on the Filtration Performance during Skim Milk Microfiltration with Flat Sheet and Spiral-Wound Membranes
by Martin Hartinger, Jonas Napiwotzki, Eva-Maria Schmid, Dominik Hoffmann, Franziska Kurz and Ulrich Kulozik
Membranes 2020, 10(4), 57; https://doi.org/10.3390/membranes10040057 - 26 Mar 2020
Cited by 9 | Viewed by 4252
Abstract
Spacer design in spiral-wound membranes (SWMs) significantly affects the axial pressure drop in the flow channel but also the deposit layer removal. However, the effects of the spacer design and feed flow distribution in the module on the filtration performance have not yet [...] Read more.
Spacer design in spiral-wound membranes (SWMs) significantly affects the axial pressure drop in the flow channel but also the deposit layer removal. However, the effects of the spacer design and feed flow distribution in the module on the filtration performance have not yet been investigated during the highly fouling-susceptible fractionation of proteins from skim milk by SWMs. Therefore, a parallel spacer with no turbulence promotion and a less homogeneous feed flow distribution in the SWM was compared to a diamond spacer with regard to its impact on deposit formation and filtration performance. The experiments were conducted in a flat sheet test cell and in SWMs. The parallel spacer induced a more homogeneous deposit layer formation. However, no difference in filtration performance could be observed in the experiments with the test cell. Even though deposit layer formation dominates the microfiltration, its amount and spatial distribution could not be directly linked to the filtration performance. Furthermore, both spacers were assessed in SWM. Despite the higher crossflow velocity applicable in the more open channels of the parallel spacer, the performance of the parallel spacer was inferior to the diamond spacer. This was independent of the viscosity of the feed. Due to the high curvature of the membrane sheets close to the permeate collection tube, the cross-section of the flow channels in the SWM equipped with the parallel spacer was reduced. This resulted in a distinctly lower deposit layer control and performance, which could not be compensated by the resulting higher crossflow velocity far from the permeate collection tube. Full article
(This article belongs to the Section Membrane Processing and Engineering)
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15 pages, 4113 KiB  
Article
Selective Separation of 1-Butanol from Aqueous Solution through Pervaporation Using PTSMP-Silica Nano Hybrid Membrane
by VSSL Prasad Talluri, Aiym Tleuova, Seyedmehdi Hosseini and Ondrej Vopicka
Membranes 2020, 10(4), 55; https://doi.org/10.3390/membranes10040055 - 26 Mar 2020
Cited by 18 | Viewed by 4168
Abstract
In this work, a poly(1-trimethylsilyl-1-propyne) (PTMSP) mixed-matrix membrane was fabricated for the selective removal of 1-butanol from aqueous solutions through pervaporation. Silica nanoparticles (SNPs), which were surface-modified with surfactant hexadecyltrimethylammonium bromide (CTAB), were incorporated into the structure of the membrane. The modified membrane [...] Read more.
In this work, a poly(1-trimethylsilyl-1-propyne) (PTMSP) mixed-matrix membrane was fabricated for the selective removal of 1-butanol from aqueous solutions through pervaporation. Silica nanoparticles (SNPs), which were surface-modified with surfactant hexadecyltrimethylammonium bromide (CTAB), were incorporated into the structure of the membrane. The modified membrane was characterized by thermogravimetry-differential scanning calorimetry (TG-DSC), contact angle measurements, and scanning electron microscope (SEM) analysis. It was found that the surface hydrophobicity of the membrane was improved when compared to neat PTMSP by contact angle measurement. It was confirmed by SEM analysis that a uniform distribution of surface-modified SNPs throughout the PTMSP membrane was achieved. The thermogravimetric analysis detected the thermal degradation of the modified PTMSP at 370 °C, which is comparable to neat PTMSP. The pervaporation measurements showed a maximum separation factor of 126 at 63 °C for 1.5 w/w% 1-butanol in the feed. The maximum total flux of approximately 1.74 mg·cm−2·min−1 was observed with the highest inspected temperature of 63 °C and at the 1-butanol concentration in the feed 4.5 w/w%. The pervaporation transients showed that the addition of the surface-modified SNPs significantly enhanced the diffusivity of 1-butanol in the composite compared to the neat PTMSP membrane. This improvement was attributed to the influence of the well-dispersed SNPs in the PTMSP matrix, which introduced an additional path for diffusivity. Full article
(This article belongs to the Special Issue Selected Papers from the MSA ECR & IMSTEC 2020)
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