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The utilization of osmosis for engineered applications sparked off various emerging technologies relying on osmotically driven membrane processes (ODMPs). Represented by forward osmosis (FO) and pressure retarded osmosis (PRO), ODMPs show great promise to leverage the global water-energy nexus and have drawn considerable attention in recent years. However, their performance in practical applications is significantly affected by membrane fouling. Membrane fouling is a complex problem and is associated with the foulant deposition, concentration polarization and reverse solute diffusion (RSD) in ODMPs. The current paper provides a comprehensive review on membrane fouling in ODMPs with a focus on the elaboration of the factors and mechanisms governing the fouling behavior. Among those fouling factors and mechanisms, some are also applicable for pressure-driven membrane processes (e.g., reverse osmosis (RO) and nanofiltration (NF)), such as the effects of hydrodynamic conditions, feedwater composition, and membrane material and properties, and the cake-enhanced concentration polarization (CE-CP) mechanism. Others are unique for ODMPs, such as the effects of draw solution composition and membrane orientation, the internal concentration polarization (ICP) self-compensation effect, and the RSD-enhanced fouling. A general osmotic-resistance filtration model for ODMPs is presented in this paper to assist in the interpretation of the intrinsic interrelationships among those fouling factors and mechanisms. The impact and mechanisms of membrane fouling on contaminates removal are also reviewed briefly based on the limited existing literature on this topic. Finally, the available membrane fouling control strategies for ODMPs are summarized upon understanding the cause and effect of fouling. Based on the current review, future research prospects are proposed for further studying the membrane fouling in ODMPs. [ABSTRACT FROM AUTHOR]

In view of the proliferating applications involving membrane-based separation, the inevitable membrane fouling phenomenon is well-studied. However, the influence of foulant shape on membrane fouling remained incompletely understood. Therefore, the goal of this study was to investigate the fouling behaviors by three different shapes of latex particles (namely, peanut, pear and sphere) with similar mean diameters in the range of 3.5–3.8 μm. External and internal fouling were studied using polycarbonate track-etched (PCTE) membranes with nominal pore sizes of 2 and 8 μm, respectively. Flux data were taken, and fouling models, optical coherence tomography (OCT) and field-emission scanning electron microscope were employed. Regarding external membrane fouling, the sphere-shaped particles displayed the worst flux decline, which is tied to the greatest tendency to deposit on the membrane pores, as revealed by the network fouling model. As for internal fouling, the flux decline curves were more similar among the particle types. The fouling model shows the sphere-shaped particles gave the densest internal cake, which caused slightly steeper flux decline in the latter part of the filtration. Furthermore, OCT indicates that the highest fouling fractions at 7.5 μm below the membrane were exhibited for the peanut-shaped particles, which is due to the preferential vertical orientation resulting in deeper penetration. Results here highlight the non-negligible influence of foulant particle shape, which warrants further understanding and accounting for membrane fouling studies. [Display omitted] • Used OCT to reveal influence of foulant particle shape on membrane fouling. • Spheres were more prone to pore-blockage and thus gave worst flux decline. • Non-spherical particles gave less dense internal cakes due to rotational effects. • Peanut-shaped particles penetrated deeper due to preferential vertical orientation. • Particle shape affected flux decline more when external fouling was dominant. [ABSTRACT FROM AUTHOR]

Membrane fouling persists to be among key obstacles in liquid membrane-based separation processes, and thereby the underlying understanding has actively been pursued. The two gaps attempted to be addressed here are namely, (i) internal fouling, which has limited studies due to limitations of instruments available; and (ii) fouling by mixtures of oppositely charged particles, as an extension to the studies on effect of surface charge of pure foulants on fouling. With the sub-micron pure constituents (namely, negatively charged carboxylated latex particles and positively charged aminated latex particles) as benchmarks, mixtures of three different compositions of the two particle types were investigated. The membrane was polycarbonate track-etched (PCTE) membrane. Surprisingly, the mixtures gave worse flux decline than that by purely positively charged aminated latex, which contradicts electrostatic considerations. The fouling model indicates that the mixtures exhibited higher pore blockage parameters (α) than either of the pure constituents, which agree with the flux decline trends. On the other hand, the mixtures gave internal cake resistance parameters (R c /R m) in between that of the pure constituents, which disagree with the fouling trends. Furthermore, optical coherence tomography (OCT) analysis indicates that the mixtures had taller buildups on the membrane as well as heterogenous internal cakes. Therefore, the steepest flux declines for the mixtures seem to be better correlated with the extensive external fouling as manifested in the taller buildups on the membrane pores, rather than internal fouling since the internal cakes were more porous. The contradictory extensive external and mitigated internal fouling phenomena are unexpected based on electrostatic considerations, and thereby highlight that fouling resulting from mixtures may not be readily extrapolated from understanding based on pure particle feeds. Image 1 • Steeper flux decline by mixtures of oppositely charged constituents than pure ones. • Mixtures gave greater pore blockage than constituents, agreeing with flux trends. • Mixtures gave intermediate internal-cake resistance, deviating from flux trends. • OCT trends affirm taller external cake and porous internal cake by mixtures. • Contradictory extensive external fouling and mitigated internal fouling by mixtures. [ABSTRACT FROM AUTHOR]

Pressure-retarded osmosis (PRO) has attracted worldwide attention for its potential applications in renewable osmotic energy harvesting, low energy seawater desalination, and industrial waste brine disposal. However, membrane fouling is one of the major issues limiting PRO performance with the use of a high-salinity draw solution and a low-value impaired feedwater. This study systematically investigated membrane fouling in the PRO process using a real wastewater retentate (a waste byproduct from wastewater reclamation plants) as the PRO feed. Organic fouling (e.g., by humic substances) and inorganic fouling (e.g., by calcium phosphate) were identified to be the major types of fouling, where the latter dominated the overall water-flux decline. The internal PRO membrane fouling was exacerbated by internal concentration polarization (ICP) and intermolecular interactions between the organic macromolecules and the scaling precursor ions (e.g., Ca 2+ ). A limiting flux that was independent of the initial flux (i.e., applied pressure) was observed during the PRO fouling and was explained by a novel PRO limiting flux model. A membrane with a smaller structural parameter could achieve a higher limiting flux in PRO. A simple and effective pressure-assisted osmotic backwashing protocol was developed to clean the internally fouled membrane that could restore over 92% of the water flux within a short cleaning period (15 mins). The PRO performance could also be significantly improved by decreasing the feedwater pH that mitigated alkaline scaling. Finally, performing the PRO membrane fouling test in the active-layer-facing-feed-solution (AL-FS) orientation revealed that the integral cellulose triacetate (CTA) membrane exhibited strong mechanical stability and anti-fouling tendency whereas the thin-film composite (TFC) membrane was not mechanically stable in this orientation. This study for the first time identified that an integral membrane instead of a TFC membrane is an excellent candidate for PRO operation in the AL-FS mode for fouling control. [ABSTRACT FROM AUTHOR]

The Derjaguin-Landau-Verwey-Overbeek (DLVO) model, as well as the extended model (XDLVO), is popularly employed to quantify the interfacial interactions underlying membrane fouling. However, disagreements between membrane fouling extent and the interaction energies derived from DLVO or XDLVO models have been reported, which suggests gaps in the understanding. This study demonstrates that the DLVO approximation methods for predicting the interfacial foulant-membrane interaction are sensitive to the boundary condition assumptions (e.g., constant charge versus constant potential). In particular, while both the Poisson-Boltzmann (P–B) and linear superposition approximation (LSA) equations can quantify the electrostatics (EL) interaction energy component, the former assumes constant potential, while the latter additionally considers constant charge scenarios. The relative accuracy of these two equations were evaluated here. For dead-end filtration tests, flux decline trends, OCT analysis results and fouling model parameters were obtained. Regarding fouling of pristine PCTE membrane by latex particles of opposite charge signs, both the P–B and LSA equations contribute to predict relative fouling extents correctly. However, for the case of the BPEI-coated membrane, the P–B equation failed whereas the LSA equation gave good agreements. For cross-flow filtration tests in organic solvents, LSA also out-performed the P–B equation in providing more accurate predictions of membrane fouling. The results here highlight the shortcomings in the commonly used P–B equation and are expected to be potentially valuable in the development of better approximations for quantifying interfacial interaction energies. [Display omitted] • Both P–B and LSA equations predict fouling of pristine membrane by latex correctly. • Only LSA predict affinity between coated membrane layer and latex correctly. • Superiority of LSA also applies to fouling in organic solvents. • P–B equation is more limited due to underlying constant-potential assumption. • Boundary condition assumptions need to be considered in use of DLVO model. [ABSTRACT FROM AUTHOR]

Membrane fouling in organic solvent environments remains poorly explored despite its significance in chemical and pharmaceutical industries. This study uses molecular dynamics (MD) simulations and experiments to explore lysozyme fouling in water, as well as four organic solvent environments, namely, 30 % v/v and 50 % v/v isopropyl alcohol (IPA), and 30 % v/v and 50 % v/v dimethyl sulfoxide (DMSO). Experimentally, flux declines were least with IPA and worst with DMSO. Biased simulations indicate the worst fouling in DMSO is tied to the most attractive lysozyme-membrane energy in the presence of DMSO. However, the relative attractive energies for IPA and water do not agree with the relative flux declines, indicating other factors are more influential when the interaction energies are similar. To understand the gentler flux decline for IPA despite the more attractive lysozyme-membrane energy, radial distribution functions (RDFs) were obtained from unbiased simulations. Analyss of the water and solvent films around both the membrane and the lysozyme molecule reveal that the denser water film around both entities induced by the presence of IPA serves as a barrier for fouling and thus leads to less flux decline. The results underscore the complexity of fouling in organic solvent systems, cautioning against direct use of the understanding based on aqueous systems. [Display omitted] • Membrane fouling by lysozyme in water, IPA and DMSO studied. • Flux decline worst in DMSO and least in IPA. • Worst fouling in DMSO tied to most significant lysozyme-membrane attraction. • Least fouling in IPA tied to denser water film around membrane and lysozyme. • Both biased and unbiased molecular dynamics simulations needed for full explanation. [ABSTRACT FROM AUTHOR]

Pressure retarded osmosis (PRO) is an innovative technique to yield osmotic energy. Nevertheless, the PRO performance is exacerbated by the severe membrane fouling occurring within the porous support. It is a potential alternative for sustainable power harvesting to change the membrane orientation from active layer facing draw solution (AL−DS) or PRO mode to active layer facing feed solution (AL−FS) or FO mode for a low-fouling propensity. A novel integral PRO hollow fiber membrane was developed in this work by phase inversion and followed with a facile cross-linking post-treatment. The structure and properties of the resultant membrane were systematically investigated using a series of characterization protocols. The PRO performance of the membrane was studied under various hydraulic pressures at the AL−FS orientation. The results reveal that the substrate with sponge-like structure and relatively dense inner surface can better withstand high pressure in PRO process. Two steps of cross-linking endowed the membrane with a smaller pore size on the outer surface that exhibits high rejection against various inorganic salts. The novel integral membrane can achieve a stable power density output around 4.3 W m −2 at 12 ~ 13 bar hydraulic pressure, using a real wastewater reverse osmosis (RO) retentate and 1.0 M sodium chloride as the feed and draw stream, correspondingly. This result demonstrates that the PRO operation in the AL−FS orientation (FO mode) offers a significant advantage over the AL−DS orientation (PRO mode) by eliminating the pretreatment of the feed water or/and other measures associated with membrane fouling control in the PRO mode. To implement the PRO operation with the AL−FS orientation, developing a robust membrane with an integral structure is critical. The newly developed integral hollow fiber membrane via chemical cross-linking presents the potential for PRO operation in the AL−FS orientation. [ABSTRACT FROM AUTHOR]

The advancement of pressure retarded osmosis (PRO) has drawn much attention recently to its feasibility of practical operation. Membrane fouling is one of the main challenges, especially when real wastewater is used as feed solution in the PRO system. Low pressure nanofiltration (NF) pretreatment was thus adopted in current study to pretreat the wastewater reverse osmosis (RO) brine collected from a wastewater treatment plant prior to feeding to the PRO process. Three NF membranes were compared in terms of the membrane properties, NF permeate (i.e., PRO feed) quality and the PRO membrane performance. Results showed that the PRO water flux could increase to 30.5 L/m 2 /h (LMH) at 16 bar applied pressure by adopting the pretreated solution using an in-house made low-pressure NF hollow fiber membrane module, in contrast to the water flux of 9 LMH for untreated wastewater RO brine. A systematic analysis of water chemistry and membrane characterization (electron dispersed X-ray (EDX) and X-ray photoelectron spectroscopy (XPS) depth profiling) revealed that calcium salts, organic compounds, and silica could be the main contributors to the membrane fouling in PRO. Low-pressure NF was able to mitigate the fouling potential from multivalent ions and organic matters, but silica scaling in PRO needs to be further addressed. [ABSTRACT FROM AUTHOR]

Increasing demand for oil and gas leads to the generation of substantial amount of produced water, bringing about deleterious impacts on the environment. Direct-contact membrane distillation (DCMD) could be a possible option for dewatering oil-in-water (O/W) emulsions because of many benefits brought by the DCMD process. However, these low surface tension solutions pose some difficult issues such as membrane fouling and pore wetting. The mechanisms involved are not fully understood due to the lack of study of the interaction between the emulsions and the membrane surface in the DCMD domain. To address the challenges, this study aims at developing a fundamental understanding of the relationship between surfactant-stabilized O/W emulsions and polyvinylidene fluoride (PVDF) membrane surface in DCMD operations. Effects of surfactant types (Span 20, Tween 20, and sodium dodecyl sulfate), oil concentration, and oil types (petroleum and vacuum pump oil) were systematically studied to better understand the fouling and wetting mechanisms involved. The results reveal that surfactant concentration and hydrophobicity had an influence on the membrane fouling and wetting behaviors. Surfactants with a lower hydrophilic-lipophilic balance (HLB) value could make the PVDF membrane surface less hydrophobic and cause less severe fouling by restraining the adsorption of oil droplets on the membrane surface. These findings suggest that membrane surface modification is required to achieve anti-fouling and anti-wetting properties to make DCMD an energy-efficient and effective technology for treating produced water. [ABSTRACT FROM AUTHOR]

Novel composite forward osmosis (FO) hollow fiber membranes with two selective skin layers were developed in the present work. The polyethersulfone (PES) hollow fiber substrate was firstly fabricated by a phase inversion method. The RO-like polyamide skin layer was then prepared on the inner surface of the hollow fiber substrate via interfacial polymerization (IP), while the NF-like outer skin layer was prepared via polyelectrolyte layer-by-layer (LBL) assembly. Three double-skinned membranes with negative (DS#1.5), positive (DS#2.0) and minimal (DS#2.5) outer surface charges under neutral pH environment were evaluated for their capabilities against organic fouling in the FO process. The newly developed double-skinned membranes possess water permeability greater than 2 l/m 2 h bar and NaCl rejection higher than 95% under 2 bar pressure, and have superior water flux and less salt leakage than the commercial HTI FO membranes as well as all the reported double-skinned FO membranes with RO-like selective layers. Most importantly, the double-skinned DS#2.5 hollow fiber membrane exhibits exciting organic fouling resistance because of its highly hydrophilic NF-like secondary layer with minimal surface charge and tightened surface structure to mitigate possible substrate pore clogging and fouling layer formation. A stable water flux of around 25 l/m 2 h was attained for DS#2.5 membrane using <0.5 M NaCl as the draw solution and a water containing 200 ppm dextran (DEX) or Aldrich humic acid (AHA), or lysozyme (LYS) and 10 mM NaCl as the model feed in the active layer against the draw solution (AL-DS) configuration, suggesting its great potential for practical FO applications. [ABSTRACT FROM AUTHOR]

The current study aimed to understand both external and internal membrane fouling by three proteins with different net charges, namely, negatively charged pepsin and bovine serum albumin (BSA), as well as positively charged lysozyme. Polycarbonate track-etched (PCTE) membranes were used. Per electrostatic attraction, the flux decline was the worst for lysozyme, which is attributed by the fouling model to the greatest pore blockage (α) and pore constriction (β), and by field-emission scanning electron microscope (FESEM) and optical coherence tomography (OCT) to the most extensive external fouling. Between pepsin and BSA, BSA gave worse flux decline despite its more negative net charge. The fouling model indicates that BSA gave greater pore blockage (α) and denser internal cake (R c / R m), while the quartz crystal microbalance with dissipation (QCM-D) indicates a rigid cake structure. Notably, despite monotonic flux decline with filtration, the OCT fouling voxel trends show significant fluctuations, which has not been reported before and thus signify the unique behavior of protein foulants in straight-through pores. Specifically, the trends below and above the −4.5 μm layer (i.e., 4.5 μm below the feed-membrane interface) are perfectly opposite, indicating the non-uniform protein deposits slipping downwards in the membrane pores as filtration progressed. The dynamic movements of the protein cakes unveiled here warrant more understanding in future studies. • Surprising fluctuations of OCT fouled voxels despite monotonically decreasing flux. • Dynamic downward motion of fouled protein deposit in the straight-through pores. • Delayed fluctuations by BSA tied to densest and most rigid cake. • Worst flux decline by lysozyme due to high pore blockage and pore constriction. [ABSTRACT FROM AUTHOR]

Membrane fouling, which is a key obstacle in implementing membrane technology, has been studied extensively for aqueous feeds. With increasing interests in organic solvent applications, a corresponding effort on understanding membrane fouling is warranted. This study employs molecular dynamics simulations to unveil the mechanisms underlying the different adsorption behaviors of dextran onto a polyacrylonitrile (PAN) membrane in three polar and protic solvents, namely, water, formamide and ethanol. The dextran-membrane separation distance is the lowest for water, followed by ethanol then formamide, which agrees with the worse flux decline for water relative to formamide observed experimentally. The greatest adsorption tendency in water is tied to the most attractive dextran-membrane interaction. On the other hand, the lower adsorption tendency in formamide and ethanol is linked to enhanced solvation of the dextran molecule and membrane, which deters dextran adsorption onto the membrane. Specifically, formamide, which leads to the least adsorption, exhibits the most attractive solvent-dextran and solvent-membrane interaction energies, the highest solvent-accessible surface area (SASA) for dextran, and also the highest density of solvent molecules in the solvation shell closest to the membrane. As for ethanol, it gives the highest density of solvent molecules in the solvation shell closest to a part of the dextran. The solvation of foulant and membrane by water deviates from that by other similarly polar and protic solvents, which has important implications in membrane fouling and highlights the need for enhancing the understanding of membrane fouling behaviors in organic solvents. [Display omitted] • Adsorption tendency of dextran on membrane is greatest in water and least in formamide. • Dextran-membrane interaction is most attractive in water. • Solvent-dextran and solvent-membrane interactions are most attractive in formamide. • Competitive solvent and dextran adsorption onto membrane governs fouling. • Greater solvation of foulant and membrane in ethanol and formamide reduces fouling. [ABSTRACT FROM AUTHOR]