Anqi, Ali E.; Usta, Mustafa; Krysko, Robert; Lee, Jung Gil; Ghaffour, NorEddine; Oztekin, Alparslan(Journal of Membrane Science, Elsevier BV, 2019-10-25)[Article]
The performance of vacuum membrane distillation (VMD) modules can be optimized through careful selection of design parameters. The present study examines how the addition of cylindrical filaments in the feed channel increases momentum mixing and the overall performance of VMD modules under different operating inlet conditions. Three-dimensional transient Computational Fluid Dynamics (CFD) simulations are conducted using Wall-Adapting Local Eddy-Viscosity (WALE) subgrid-scale Large Eddy Simulation (LES) turbulence model. Local concentration, temperature, and flux are coupled at the membrane surface to predict the rate of water vapor diffused through the membrane by Knudsen and viscous diffusion mechanisms. The predicted and measured vapor flux agrees reasonably well; validating the employed model. The small-scale eddies induced by the presence of spacer filaments promote mixing in the module, thus the temperature and concentration polarization is alleviated and the water vapor flux is immensely improved. The insertions of filaments in the feed channel increase the water permeate rate by more than 50% at higher feed flow rates and inlet temperatures. The pressure drop by the spacer reduces the allowable module length by one order of magnitude, but the module length increases two folds at feed temperature 80℃. Even though the power consumption of the module containing the filaments is increased, the addition of filaments is strongly recommended since the required power for the process could be supplied from readily available low-grade heat source.
Falca, Gheorghe; Musteata, Valentina-Elena; Behzad, Ali Reza; Chisca, Stefan; Nunes, Suzana Pereira(Journal of Membrane Science, Elsevier BV, 2019-05-08)[Article]
Cellulose is the most abundant biopolymer, but it is difficult to process due to its low solubility in most of the solvents. In this work, we demonstrate the preparation, of self-standing and defect-free cellulose hollow fiber membranes made by a sustainable process for filtration in organic solvent medium. The hollow fibers were made by the simple spinning technique using ionic liquids as a solvent. The spun solutions were prepared with three different ionic liquids, having imidazolium-based cations and acetate or phosphates as anions. We used X-ray diffraction to evaluate the influence of the different ionic liquids on the crystallinity of the cellulose and the membrane solvent stability. We used cryo-scanning electron microscopy to investigate the porous structure of the hydrated membranes, distinguishing it from that of the dry membranes. The hollow fiber membrane performance was studied using dyes in water and ethanol solutions. The rejection of Congo Red (696 g mol−1) was higher than 90% in ethanol and even closer to 100% in water. The best results were obtained by using 1-ethyl-3-methyimidazolium diethyl phosphate and 1,3-dimethylimidazolium dimethyl phosphate. Our results indicate that by using greener process is possible to obtain solvent resistant cellulose hollow fibers.
Guo, Jiaxin; Lee, Jung Gil; Tan, Tian; Yeo, Joonho; Wong, Pak Wai; Ghaffour, Noreddine; An, Alicia Kyoungjin(Journal of Membrane Science, Elsevier BV, 2019-07-17)[Article]
Removing nitrogen from wastewater by conventional treatment methods requires substantial energy, only to release it back to the atmosphere as gaseous nitrogen. Herein, we investigated the applicability of membrane distillation (MD) in resource recovery from sludge digestate by controlling the volatility and pressure of the vapor transport across the membrane to concentrate ammonia in the permeate stream. A mixture of Nafion ionomer and Multiwall Carbon Nanotubes (MWCNTs) were incorporated into a Poly (vinylidene fluoride-co-hexafluoropropene; PVDF-HFP) nanofiber matrix to fabricate a nanoporous honeycomb Nafion membrane featuring high recovery and increased mechanical strength. Theoretical modeling was conducted to predict the expected performance of the fabricated Nafion membrane under different operation conditions and to reveal the mechanism behind the enhanced recovery of Nafion membranes in the MD process. The resultant Nafion (8%)/MWCNT (2.5%)/PVDF-HFP nanofibrous membrane showed up to three times higher ammonia recovery compared to the commercial PVDF membrane from a feed with an ammonia concentration of 300 mg/L. The theoretical analysis quantitatively revealed that the Nafion containing membrane can not only suppress the negative effect of membrane's structural resistance on the ammonia recovery efficiency but also enhance the efficiency. In addition, we also uncovered that the effect of Nafion on ammonia recovery efficiency was maximized when the Nafion 8% membrane was employed. This study demonstrated an innovative and realistically applicable MD treatment process for recovering resource, which integrates low-grade heat and has scaling-up potential for wastewater treatment plants.
Qamar, Adnan; Bucs,Szilard; Picioreanu, Cristian; Vrouwenvelder, Johannes S.; Ghaffour, Noreddine(Journal of Membrane Science, Elsevier BV, 2019-07-19)[Article]
A vital component of spiral-wound membrane modules is the spacer mesh. It not only structurally supports the membranes but also aids in mass-transport enhancement through the membrane surface. Fundamental understanding of hydrodynamics associated with these spacer designs is critical to improve the permeate flux performance by decreasing concentration polarization and minimizing (bio)fouling, as well as minimizing the axial pressure drop. In the present study, time and space resolved Direct Numerical Simulations (DNS) were performed for a commercial spacer geometry. The spacer geometry was reconstructed by measurements using Scanning Electron Microscopy (SEM). Computations were performed for three spacer cells, allowing elimination of stream-wise periodicity that was a major bottleneck in earlier studies. The numerical solver was well checked in terms of boundary layer profiles obtained from Particle Image Velocimetry (PIV) data and with pressure measurements corresponding to various flow channel velocities. Non-dimensional computations were performed for Reynolds Numbers (Re) ranging from 73 to 375 (inlet channel velocity of 0.073–0.375 m/s) covering the flow transition dynamics regime. Results indicate that flow transition from steady to unsteady regime occurs for Re > 250. The flow transition could be primarily attributed to the interaction between vortices attached to the spacer filaments and the screw-vortex that originates along the diagonal of the spacer cells. No turbulent transition was observed even at the highest investigated velocity (Re = 375). The frequency spectra of time-varying velocity signal shows that at Re > 350 a sudden shift of frequency spectra occurs from discrete to continuous mode indicating the onset of advanced instability. Spacer design criteria in terms of maximum principal stress is also proposed, which can potentially aid in minimizing biofilm seeding.
Siebdrath, Nadine; Siddiqui, Amber; Ding, Wei; Kruithof, Joop; Vrouwenvelder, Johannes S.(Journal of Membrane Science, Elsevier BV, 2019-05-18)[Article]
Biofouling development is affected by a variety of factors that change over the length of reverse osmosis (RO) membrane modules in pressure vessels. Spatially resolved biofouling formation was studied under conditions representative to practice using four one-meter Long Channel Membrane Test Cells (LCMTCs) in series, simulating an industrial pressure vessel.
Biofouling was induced by dosing an easily assimilable substrate to the feed water. The impact of biofouling on the sequential decline of RO membrane performance indicators (feed channel pressure drop, permeability and salt rejection) was investigated. Also, the temporal organic carbon (DOC) consumption was assessed spatially over the four test cells.
Results showed that all membrane performance indicators were impacted by biofouling formation. The feed channel pressure (FCP) drop increase was impacted earliest and strongest followed by permeability and salt rejection decline, underlining that FCP drop is a sensitive and early biofouling monitoring indicator. Spatially resolved biofouling investigations revealed that most biofouling was formed in the lead sections of membrane installation with a decreasing gradient over length, linked to DOC availability in the system. In this study, FCP drop played a crucial role: the FCP drop increase at the lead test cell of the membrane installation caused performance losses for the downstream test cells.
Minimizing the effect of biofouling on membrane performance should be pursued by a combination of strategies involving (i) early detection and preventive cleaning, (ii) substrate limitation for delaying biofouling built-up and (iii) optimized (early) cleaning procedures for more effective biofilm removal.
A highly contorted, carbon-rich intrinsically microporous polyimide (PIM-PI) made from spirobifluorene dianhydride and 3,3-dimethylnaphthidine (SBFDA-DMN) was employed as a precursor for the formation of carbon molecular sieve (CMS) membranes at pyrolysis temperatures from 550 to 1000 °C. The high carbon content of SBFDA-DMN (∼84%) resulted in only 28% total weight loss during pyrolysis under a nitrogen atmosphere at 1000 °C. The development of the various microstructural textures was characterized by gas sorption analysis, Brunauer-Emmett-Teller (BET) surface area, X-ray diffraction, Raman spectroscopy, electrical conductivity, and gas transport properties. Heat treatment of a pristine SBFDA-DMN membrane at 550 °C resulted in reduced permeability for all gases (e.g.: PCO2 dropped from 4700 to 1500 barrer) as well as lower BET surface area from 621 to 545 m2 g−1. At 600 °C, new pores induced by pyrolysis increased the BET surface area to nearly that of the precursor and significantly improved gas separation performance. Above 600 °C, a progressive collapse of the micropores became evident with CMS membranes showing higher gas-pair selectivity but lower permeability. At 1000 °C, ultra-micropores comparable in size with the kinetic diameter of CH4 emerged and induced a prominent molecular sieving effect resulting in very high CH4 rejection. This strong size exclusion effect, further supported by gravimetric gas sorption measurements, resulted in unusually high N2/CH4 and CO2/CH4 selectivities of 35 and 1475, respectively.
We developed composite membranes by stacking functionalized nanospheres (20 nm size) with a high density of H-bonds. The functionalized nanospheres were formed by a click-reaction in toluene between the polybutadiene segment of poly(styrene-b-butadiene-b-styrene) (PS-b-PB-b-PS) triblock copolymer and an azodicarbonyl (PTAD) compound. The strong hydrogen-bond interaction promoted by the pendant urazole groups of the PTAD-modified copolymer is an important parameter for obtaining stable and defect-free membranes, acting in analogy to self-healing systems. The hydrodynamic transport is facilitated by the high porosity of the membranes and the unique hourglass-shaped pores. The composite membrane has water permeation as high as 60 L m−2 h−1 bar−1 and can exclude more than 95% of proteins with a molecular weight as small as 12 kg mol−1. This novel class of nanoparticle-stacked membranes has therefore excellent separation properties for biomolecular separation.
Akther, Nawshad; Phuntsho, Sherub; Chen, Yuan; Ghaffour, NorEddine; Shon, Ho Kyong(Journal of Membrane Science, Elsevier BV, 2019-05-08)[Article]
Polyamide thin-film composite (PA TFC) membranes have attained much attention for forward osmosis (FO) applications in separation processes, water and wastewater treatment due to their superior intrinsic properties, such as high salt rejection and water permeability compared to the first-generation cellulose-based FO membranes. Nonetheless, several problems like fouling and trade-off between membrane selectivity and water permeability have hindered the progress of conventional PA TFC FO membranes for real applications. To overcome these issues, nanomaterials or chemical additives have been integrated into the TFC membranes. Nanomaterial-modified membranes have demonstrated significant improvement in their anti-fouling properties and FO performance. In addition, the PA TFC membranes can be designed for specific applications like heavy metal removal and osmotic membrane bioreactor by using nanomaterials to modify their physicochemical properties (porosity, surface charge, hydrophilicity, membrane structure and mechanical strength). This review provides a comprehensive summary of the progress of nanocomposite PA TFC membrane since its first development for FO in the year 2012. The nanomaterial-incorporated TFC membranes are classified into four categories based on the location of nanomaterial in/on the membranes: embedded inside the PA active layer, incorporated within the substrate, coated on the PA layer surface, or deposited as an interlayer between the substrate and the PA active layer. The key challenges still being confronted and the future research directions for nanocomposite PA TFC FO are also discussed.
In the present work, a convenient and direct technique which enables to characterize the intrinsic structure and the mechanical properties of the biofilm without altering its chemical and physical properties is proposed. By utilizing the Optical Coherence Tomography (OCT) as a structural imaging tool coupled with an advance mathematical framework, thickness, micro-porosity, normal stress-strain curve, bulk modulus and total permeability of the biofilm structures are determined. The accuracy of this mathematical technique for the in situ characterization is validated by analyzing two different membrane structures for porosity and permeability values against the mercury intrusion porosimetry method. Three-dimensional images of biofouling were obtained with high resolution aided to numerically analyze the intrinsic biofilm structure at microscale. Growth of biofilm in a dead-end filtration experimental setup was investigated by varying the feed flow rate which allowed uniform compression and decompression to compute normal stress-strain relation of the evolving biofilm structure. At early development of biofilm (day 3), the thickness and normal stress/strain curve showed that the biofilm structure behave similar to elastic material. However, hysteresis-like trend starts to appear with the growth of biofilm suggesting the deviation of biofilm properties to viscoelastic nature at day 8. The microstructure porosity increased from 0.214 (day 3) to 0.482 (day 8) at a feed flow rate of 15 mL/min. The total membrane/biofilm permeability decreased with biofilm age to reach 5.19 × 10−15 m2 at day 8 at the same flow rate, leading to a reduction of permeate flux over time. All the structural properties were found to be time dependent as the biofilm continuously evolved.
The state of the art membrane chemistry for reverse osmosis application is based on a classical interfacial polymerization reaction between a diamine in the aqueous phase and trifunctional acid chloride in the organic phase. Because of the very fast reaction rate of the interfacial polymerization, the extremely thin nature (typically ≤200 nm), and the insolubility of the resulting polyamide layer, the conversion rate has not been directly studied. In this work, high field (21.2 T) solid state NMR was utilized to directly measure amide to amine ratio of the polyamide layers in commercial RO membrane. Contrary to earlier indirect measurement, amines are rather abundant in these polyamide layers. Because of the dramatic reactant concentration differences on the opposing surfaces of the growing membrane, compositional heterogeneity is expected to exist across the membrane thickness. Dynamic nuclear polarization combined with solid-state NMR was utilized to probe the amide to amine ratio close to the membrane surface and was successful in differentiating membrane targeting different end user applications. The findings are important to understand both the interfacial polymerization chemistry as well as the performance of the resulting RO membrane since the amine groups present can form hydrogen bonds and ionize or deionize based on pH. The surface amine groups can be further chemically modified to acquire additional properties for membranes.
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