Preparation of Superhydrophilic and Underwater Superoleophobic Nanofiber-Based Meshes from Waste Glass for Multifunctional Oil/Water Separation.

The deterioration of water resources due to oil pollution, arising from oil spills, industrial oily wastewater discharge, etc., urgently requires the development of novel functional materials for highly efficient water remediation. Recently, superhydrophilic and underwater superoleophobic materials have drawn significant attention due to their low oil adhesion and selective oil/water separation. However, it is still a challenge to prepare low-cost, environmentally friendly, and multifunctional materials with superhydrophilicity and underwater superoleophobicity, which can be stably used for oil/water separation under harsh working conditions. Here, the preparation of nanofiber-based meshes derived from waste glass through a green and sustainable route is demonstrated. The resulting meshes exhibit excellent performance in the selective separation of a wide range of oil/water mixtures. Importantly, these meshes can also maintain the superwetting property and high oil/water separation efficiency under various harsh conditions. Furthermore, the as-prepared mesh can remove water-soluble contaminants simultaneously during the oil/water separation process, leading to multifunctional water purification. The low-cost and environmentally friendly fabrication, harsh-environment resistance, and multifunctional characteristics make these nanofiber-based meshes promising toward oil/water separation under practical conditions.

Recent Development of Advanced Materials with Special Wettability for Selective Oil/Water Separation.

The increasing number of oil spill accidents have a catastrophic impact on our aquatic environment. Recently, special wettable materials used for the oil/water separation have received significant research attention. Due to their opposing affinities towards water and oil, i.e., hydrophobic and oleophilic, or hydrophilic and oleophobic, such materials can be used to remove only one phase from the oil/water mixture, and simultaneously repel the other phase, thus achieving selective oil/water separation. Moreover, the synergistic effect between the surface chemistry and surface architecture can further promote the superwetting behavior, resulting in the improved separation efficiency. Here, recently developed materials with special wettability for selective oil/water separation are summarized and discussed. These materials can be categorized based on their oil/water separating mechanisms, i.e., filtration and absorption. In each section, representative studies will be highlighted, with emphasis on the materials wetting properties and innovative aspects. Finally, challenges and future research directions in this emerging and promising research field will be briefly described.

Application of Hollow Fiber Forward Osmosis Membranes for Produced and Process Water Volume Reduction: An Osmotic Concentration Process.

Produced and process water (PPW) from oil and gas operations, specifically in Qatar, are disposed of by deep well injection in onshore facilities. Disposing large volumes of PPW may affect deep well formation sustainability highlighting the need for effective PPW management. Forward osmosis (FO) was applied as an "osmotic concentration" process to reduce PPW injection volumes by 50% using brines and seawater as draw solutions (DS). The energy intensive step of restoring the salinity of the DS was eliminated; the diluted DS would be simply discharged to the ocean. Both hollow fiber and flat sheet FO membranes were tested and the former exhibited better flux and rejection; they are the focus of this study. Optimization experiments, conducted using Box-Behnken statistical design, confirmed that temperature and DS concentration had a substantial effect on performance. To validate the concept, a long-term experiment, under optimized conditions, was conducted with PPW as feed and brine from thermal desalination plant as DS which yielded an average flux of 24 L/m(2)h. The results confirmed that low-energy osmotic concentration FO has the potential for full-scale implementation to reduce PPW injection volumes. Pilot testing opportunities are being evaluated to demonstrate the effectiveness of this technology under field conditions.

Analyzing the Evolution of Membrane Fouling via a Novel Method Based on 3D Optical Coherence Tomography Imaging.

The development of novel tools for studying the fouling behavior during membrane processes is critical. This work explored optical coherence tomography (OCT) to quantitatively interpret the formation of a cake layer during a membrane process; the quantitative analysis was based on a novel image processing method that was able to precisely resolve the 3D structure of the cake layer on a micrometer scale. Fouling experiments were carried out with foulants having different physicochemical characteristics (silica nanoparticles and bentonite particles). The cake layers formed at a series of times were digitalized using the OCT-based characterization. The specific deposit (cake volume/membrane surface area) and surface coverage were evaluated as a function of time, which for the first time provided direct experimental evidence for the transition of various fouling mechanisms. Axial stripes were observed in the grayscale plots showing the deposit distribution in the scanned area; this interesting observation was in agreement with the instability analysis that correlated the polarized particle groups with the small disturbances in the boundary layer. This work confirms that the OCT-based characterization is able to provide deep insights into membrane fouling processes and offers a powerful tool for exploring membrane processes with enhanced performance.

Nitric oxide treatment for the control of reverse osmosis membrane biofouling.

Biofouling remains a key challenge for membrane-based water treatment systems. This study investigated the dispersal potential of the nitric oxide (NO) donor compound, PROLI NONOate, on single- and mixed-species biofilms formed by bacteria isolated from industrial membrane bioreactor and reverse osmosis (RO) membranes. The potential of PROLI NONOate to control RO membrane biofouling was also examined. Confocal microscopy revealed that PROLI NONOate exposure induced biofilm dispersal in all but two of the bacteria tested and successfully dispersed mixed-species biofilms. The addition of 40 µM PROLI NONOate at 24-h intervals to a laboratory-scale RO system led to a 92% reduction in the rate of biofouling (pressure rise over a given period) by a bacterial community cultured from an industrial RO membrane. Confocal microscopy and extracellular polymeric substances (EPS) extraction revealed that PROLI NONOate treatment led to a 48% reduction in polysaccharides, a 66% reduction in proteins, and a 29% reduction in microbial cells compared to the untreated control. A reduction in biofilm surface coverage (59% compared to 98%, treated compared to control) and average thickness (20 µm compared to 26 µm, treated compared to control) was also observed. The addition of PROLI NONOate led to a 22% increase in the time required for the RO module to reach its maximum transmembrane pressure (TMP), further indicating that NO treatment delayed fouling. Pyrosequencing analysis revealed that the NO treatment did not significantly alter the microbial community composition of the membrane biofilm. These results present strong evidence for the application of PROLI NONOate for prevention of RO biofouling.

Bactericidal mechanisms revealed for rapid water disinfection by superabsorbent cryogels decorated with silver nanoparticles.

The authors have recently reported the fabrication of superabsorbent cryogels decorated with silver nanoparticles (PSA/AgNP cryogels) that demonstrate rapid water disinfection. This paper provides a systematic elucidation of the bactericidal mechanisms of AgNPs (silver nanoparticles), both generally and in the specific context of cryogels. Direct contact between the PSA/AgNP cryogel interface and the bacterial cells is required to accomplish disinfection. Specifically, the disinfection efficacy is closely correlated to the cell-bound Ag concentration, which constitutes >90% of the Ag released. Cells exposed to PSA/AgNP cryogels show a significant depletion of intracellular adenosine triphosphate (ATP) content and cell-membrane lesions. A positive ROS (reactive oxygen species) scavenging test confirms the involvement of ROS (·O2(-), H2O2, and ·OH) in the bactericidal mechanism. Furthermore, exposed bacterial cells show an enhanced level of thiobarbituric acid reactive substances, indicating the occurrence of cell-membrane peroxidation mediated by ROS. In addition, this study reveals that both Ag(+) and Ag(0) are involved in the bactericidal mechanism of AgNPs via tests conducted using PSA cryogels with bound Ag(+) ions (or PSA/Ag(+) cryogels without reducing Ag(+) to Ag(0)). Significantly, bacterial cells exposed to PSA/Ag(+) cryogels did not show any cell-membrane damage even though the former had a higher cell-bound Ag concentration than that of the PSA/AgNP cryogels, thus indicating the differential action of Ag(+) and Ag(0).

Characterization of the archaeal community fouling a membrane bioreactor.

Biofilm formation, one of the primary causes of biofouling, results in reduced membrane flux or increased transmembrane pressure and thus represents a major impediment to the wider implementation of membrane bioreactor (MBR) technologies for water purification. Most studies have focused on the role of bacteria in membrane fouling as they are the most dominant and best studied organisms present in the MBR. In contrast, there is limited information on the role of the archaeal community in biofilm formation in MBRs. This study investigated the composition of the archaeal community during the process of biofouling in an MBR. The archaeal community was observed to have lower richness and diversity in the biofilm than the sludge during the establishment of biofilms at low transmembrane pressure (TMP). Clustering of the communities based on the Bray-Curtis similarity matrix indicated that a subset of the sludge archaeal community formed the initial biofilms. The archaeal community in the biofilm was mainly composed of Thermoprotei, Thermoplasmata, Thermococci, Methanopyri, Methanomicrobia and Halobacteria. Among them, the Thermoprotei and Thermoplasmata were present at higher relative proportions in the biofilms than they were in the sludge. Additionally, the Thermoprotei, Thermoplasmata and Thermococci were the dominant organisms detected in the initial biofilms at low TMP, while as the TMP increased, the Methanopyri, Methanomicrobia, Aciduliprofundum and Halobacteria were present at higher abundances in the biofilms at high TMP.

Synthetic membranes for water purification: status and future.

Membrane technology offers the best options to "drought proof" mankind on an increasingly thirsty planet by purifying seawater or used (waste) water. Although desalination by reverse osmosis (RO) and wastewater treatment by membrane bioreactors are well established the various membrane technologies still need to be significantly improved in terms of separation properties, energy demand and costs. We can now define the ideal characteristics of membranes and advances in material science and novel chemistries are leading to increasingly effective membranes. However developments in membranes must be matched by improved device design and membrane engineering. It is likely that limitations in fluid mechanics and mass transfer will define the upper bounds of membrane performance. Nevertheless major advances and growth over the next 20 years can be anticipated with RO remaining as the key to desalination and reclamation, with other membrane processes growing in support and in niche areas.

Fabrication of bioinspired composite nanofiber membranes with robust superhydrophobicity for direct contact membrane distillation.

The practical application of membrane distillation (MD) for water purification is hindered by the absence of desirable membranes that can fulfill the special requirements of the MD process. Compared to the membranes fabricated by other methods, nanofiber membranes produced by electrospinning are of great interest due to their high porosity, low tortuosity, large surface pore size, and high surface hydrophobicity. However, the stable performance of the nanofiber membranes in the MD process is still unsatisfactory. Inspired by the unique structure of the lotus leaf, this study aimed to develop a strategy to construct superhydrophobic composite nanofiber membranes with robust superhydrophobicity and high porosity suitable for use in MD. The newly developed membrane consists of a superhydrophobic silica-PVDF composite selective skin formed on a polyvinylidene fluoride (PVDF) porous nanofiber scaffold via electrospinning. This fabrication method could be easily scaled up due to its simple preparation procedures. The effects of silica diameter and concentration on membrane contact angle, sliding angle, and MD performance were investigated thoroughly. For the first time, the direct contact membrane distillation (DCMD) tests demonstrate that the newly developed membranes are able to present stable high performance over 50 h of testing time, and the superhydrophobic selective layer exhibits excellent durability in ultrasonic treatment and a continuous DCMD test. It is believed that this novel design strategy has great potential for MD membrane fabrication.

Novel approach to characterizing the growth of a fouling layer during membrane filtration via optical coherence tomography.

Fouling control is one of the critical issues in membrane filtration and plays a very important role in water/wastewater treatment. Better understanding of the underlying fouling mechanisms entails novel characterization techniques that can realize a real-time noninvasive observation and provide high resolution images recording the formation of a fouling layer. This work presents a characterization method based on optical coherence tomography (OCT), which is able to detect the internal structures and motions by analyzing the interference signals. An OCT system was incorporated with a laboratory-scale membrane filtration system, and the growth of the fouling layer was observed by using the structural imaging. Taking advantage of the Doppler effects, the OCT-based characterization also provided the velocity profiles of the fluid field, which are of great value in analyzing the formation of the cake layer. The characterization results clearly reveal for the first time the evolution of the morphology of the cake layer under different microhydrodynamic environments. This study demonstrates that OCT-based characterization is a powerful tool for investigating the dynamic processes during membrane fouling.

The correlation between biofilm biopolymer composition and membrane fouling in submerged membrane bioreactors.

Biofouling, the combined effect of microorganism and biopolymer accumulation, significantly reduces the process efficiency of membrane bioreactors (MBRs). Here, four biofilm components, alpha-polysaccharides, beta-polysaccharides, proteins and microorganisms, were quantified in MBRs. The biomass of each component was positively correlated with the transmembrane pressure increase in MBRs. Proteins were the most abundant biopolymer in biofilms and showed the fastest rate of increase. The spatial distribution and co-localization analysis of the biofouling components indicated at least 60% of the extracellular polysaccharide (EPS) components were associated with the microbial cells when the transmembrane pressure (TMP) entered the jump phase, suggesting that the EPS components were either secreted by the biofilm cells or that the deposition of these components facilitated biofilm formation. It is suggested that biofilm formation and the accumulation of EPS are intrinsically coupled, resulting in biofouling and loss of system performance. Therefore, strategies that control biofilm formation on membranes may result in a significant improvement of MBR performance.

Effects of proteoliposome composition and draw solution types on separation performance of aquaporin-based proteoliposomes: implications for seawater desalination using aquaporin-based biomimetic membranes.

Aquaporins are a large family of water transport proteins in cell membranes. Their high water permeability and solute rejection make them potential building blocks for high-performance biomimetic membranes for desalination. In the current study, proteoliposomes were prepared using AquaporinZ from Escherichia coli cells, and their separation properties were characterized by stopped-flow measurements. The current study systematically investigated the effect of proteoliposome composition (lipid type, protein-to-lipid ratio (PLR), and the addition of cholesterol) on water permeability and NaCl retention. Among the various lipids investigated, 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC)-based proteoliposomes were found to have excellent osmotic water permeability and NaCl reflection coefficient values. Increasing the PLR of DOPC proteoliposomes up to 1:200 increased their osmotic water permeability. However, further increase in the PLR reduced the osmotic water permeability probably due to the occurrence of defects in the proteoliposomes, whereas the addition of cholesterol improved their osmotic water permeation likely due to defects sealing. The current study also investigated the effect of major dissolved ions in seawater (e.g., Mg(2+) and SO(4)(2-)) on the stability of proteoliposomes, and design criteria for aquaporin-based biomimetic membranes are proposed in the context of desalination.

Superabsorbent cryogels decorated with silver nanoparticles as a novel water technology for point-of-use disinfection.

This paper reports the preparation of poly(sodium acrylate) (PSA) cryogels decorated with silver nanoparticles (AgNPs) for point-of-use (POU) water disinfection. The PSA/Ag cryogels combine the high porosity, excellent mechanical and water absorption properties of cryogels, and uniform dispersion of fine AgNPs on the cryogel pore surface for rapid disinfection with minimal Ag release (<100 µg L(-1)). They were used in a process that employed their ability to absorb water, which subsequently could be released via application of mild pressure. Their antibacterial performance was evaluated based on the disinfection efficacies of E. coli and B. subtilis . The PSA/Ag cryogels had excellent disinfection efficacies showing close to a 3 log reduction of viable bacteria after a brief 15 s contact time. They were highly reusable as there was no significant difference in the disinfection efficacies over five cycles of operation. The biocidal action of the PSA/Ag cryogels is believed to be dominated by surface-controlled mechanisms that are dependent on direct contact of the interface of PSA/Ag cryogels with the bacterial cells. The PSA/Ag cryogels are thought to offer a simpler approach for drinking water disinfection in disaster relief applications.

Dynamics of biofilm formation under different nutrient levels and the effect on biofouling of a reverse osmosis membrane system.

Pseudomonas aeruginosa PAO1 wild type and a mucoid derivative (FRD1) which over produces alginate were used to foul reverse osmosis (RO) membranes. When operated at a constant flux, biofilm formation on the RO membrane resulted in a slow rise in transmembrane pressure (TMP) of 22% for the initial four days of operation, followed by a sharp increase of 159% over the following two days. The initial slow increase in TMP was probably due to the formation of a biofilm on the membrane surface, which then accelerated the rate of biofouling through the effect of concentration polarization. At later stages of operation, most of the bacterial biomass consisted of dead cells. The amount of extracellular polymeric substances appeared to correlate positively with the number of dead cells. The results indicate that prolonging the initial stage of slow TMP increase and avoiding the latter stage of accelerated TMP increase would provide a sustainable operation of the RO system. These results suggest that nutrient limitation could reduce biofilm accumulation and delay the increase in TMP.

Enhanced biodegradation of 4-aminobenzenesulfonate in membrane bioreactor by Pannonibacter sp. W1.

4-Aminobenzenesulfonate (4-ABS), an aromatic amine and recalcitrant toxic pollutant, is widely used in the dye and pharmaceutical industry. Pannonibactersp. W1 is a specialized microbial strain which can efficiently degrade 4-ABS. This study shows the feasibility of using the specialized strain in an MBR system to treat synthetic wastewater containing large amount of 4-ABS. Due to membrane retention, the biomass concentration is able to reach 5 g/L within two months of continuous operation. Pannonibacter sp. W1 is able to adapt to the high loading rate of 1000 mg 4-ABS/L and achieve a remarkable 4-ABS removal efficiency of 99% within 6 h. Strain W1 grows well under the MBR continuous operation and remains as the dominant bacterium at the end of 60 days continuous operation. Minor membrane fouling has been detected within 40 days of operating at 15 LMH. At a flux of 25 LMH, the system experiences the 'TMP jump'. The high organic removal rate and low membrane fouling results illustrate the excellent performance of the bioaugmented MBR system in 4-ABS wastewater treatment.

Mitigation of membrane particulate fouling by nano/microplastics via physical cleaning strategies.

Membrane fouling by nano/microplastics (NP/MPs) is an emerging concern threatening the performance of water and wastewater treatment facilities. The NP/MPs can lead to surface adsorption, fouling and potential mechanical abrasion of the membranes. In this work, periodic gas scouring was applied during the filtration of nano/microplastics across ultrafiltration membranes to investigate the impact of shear forces on the adsorption of nano/microplastics. A series of surface energy and chemistry-modified membranes were also used including acrylic acid, cyclopropylamine and hexamethyldisiloxane plasma-modified membranes, allowing for a set of materials with controlled hydrophilicity, roughness and surface charge. Bubbling gas within the system at a gas flow rate of 0.5 to 1 L·min-1 and a water flow rate of 2 L·min-1 was found to limit the water flux decline across the pristine and hydrophobic membranes compared to the filtration experiments performed without cleaning from 38 to 22 and 23%, respectively. The adsorption of nano/microplastics onto the surface of the membranes was also simultaneously decreased from 40 to 25 and 19%, respectively. Interestingly, for the hydrophilised membranes no enhancement in permeance was observed when performing gas scouring due to the already low tendency for selective adsorption of the nano/microplastics onto their surface. The correlation of a dimensionless fouling number to the shear stress number suggested that the shear forces induced by gas scouring reduced nano/microplastics adsorption up to a gas injection ratio (volume fraction of gas) of 0.3, where the wall shear stress at the surface of the membrane was limited. This work offers an advanced physical strategy to reduce and control membrane fouling by nano/microplastics, with potential for this strategy to be adapted for more complex water matrices and plastic particles.

Optimization of Aquaporin Loading for Performance Enhancement of Aquaporin-Based Biomimetic Thin-Film Composite Membranes.

The aquaporin-based biomimetic thin-film composite membrane (ABM-TFC) has demonstrated superior separation performance and achieved successful commercialization. The larger-scale production of the ABM membrane requires an appropriate balance between the performance and manufacturing cost. This study has systematically investigated the effects of proteoliposome concentration, protein-to-lipid ratio, as well as the additive on the separation performance of ABM for the purpose of finding the optimal preparation conditions for the ABM from the perspective of industrial production. Although increasing the proteoliposome concentration or protein-to-lipid ratio within a certain range could significantly enhance the water permeability of ABMs by increasing the loading of aquaporins in the selective layer, the enhancement effect was marginal or even compromised beyond an optimal point. Alternatively, adding cholesterol in the proteoliposome could further enhance the water flux of the ABM membrane, with minor effects on the salt rejection. The optimized ABM not only achieved a nearly doubled water flux with unchanged salt rejection compared to the control, but also demonstrated satisfactory filtration stability within a wide range of operation temperatures. This study provides a practical strategy for the optimization of ABM-TFC membranes to fit within the scheme of industrial-scale production.

Surface modification of nanofiltration membranes to improve the removal of organic micropollutants: Linking membrane characteristics to solute transmission.

Surface modification of nanofiltration (NF) membranes has great potential to improve the removal of organic micropollutants (OMs) by NF membranes. This study used polydopamine (PDA) as a model coating to comprehensively link the changes in membrane properties with the changes in transmission of 34 OMs. The membrane characterization demonstrated that a thicker, denser, and more hydrophilic PDA coating can be achieved by increasing the PDA deposition time from 0.5 to 4 hours. Overall, the transmissions of target OMs were reduced by PDA-coated NF membranes compared to unmodified NF membranes. The neutral hydrophobic compounds showed lower transmissions for longer PDA coating (PDA4), while the neutral hydrophilic compounds tended to show lower transmissions for shorter PDA coating (PDA0.5). To explain this, competing effects provided by the PDA coatings are proposed including sealing defects, inducing cake-enhanced concentration polarization in the coating layer for neutral hydrophilic compounds, and weakened hydrophobic adsorption for neutral hydrophobic compounds. For charged compounds, PDA4 with the greatest negative charge among the PDA-coated membranes showed the lowest transmission. Depending on the molecular size and hydrophilicity of the compounds, the transmission of OMs by the PDA4 coating could be reduced by 70% with only a 26.4% decline in water permeance. The correlations and mechanistic insights provided by this work are highly useful for designing membranes with specific surface properties via surface modification to improve the removal of OMs without compromising water production.

Direct microscopic observation of forward osmosis membrane fouling.

This study describes the application of a noninvasive direct microscopic observation method for characterizing fouling of a forward osmosis (FO) membrane. The effect of the draw solution concentration, membrane orientation, and feed spacer on FO fouling was systematically investigated in a cross-flow setup using latex particles as model foulant in the feedwater. Higher draw solution (DS) concentrations (and thus increased flux levels) resulted in dramatic increase in the surface coverage by latex particles, suggesting that the critical flux concept might be applicable even for the osmotically driven FO process. Under identical draw solution concentrations, the active-layer-facing-the-feed-solution orientation (AL-FS) experienced significantly less fouling compared to the alternative orientation. This may be explained by the lower water flux in AL-FS, which is consistent with the critical flux concept. The use of a feed spacer not only dramatically enhanced the initial flux of the FO membrane, but also significantly improved the flux stability during FO fouling. Despite such beneficial effects of using the feed spacer, a significant amount of particle accumulation was found near the spacer filament, suggesting further opportunities for improved spacer design. To the best of the authors' knowledge, this is the first direct microscopic observation study on FO fouling.

Fouling propensity of forward osmosis: investigation of the slower flux decline phenomenon.

Forward Osmosis (FO) is a membrane process that uses the natural osmotic pressure of a concentrated draw solution to extract pure water from a feed stream. The attraction of the FO process is that it uses dense membranes, while operating at ambient pressure. This means that the FO process could potentially produce high quality water with lower energy consumption, as compared to the other desalination or reclamation processes. As FO does not entail the use of hydraulic pressure, FO has been hypothesized to have lower fouling propensity than pressure driven membrane processes. Membrane fouling has significant impact on the operational sustainability and economics of the process. This study examines the possible contributing factors to the slower flux decline observed in FO experiments based on a combined experimental and modelling approach. It was found that these factors could include low water fluxes, use of hydrophilic and smooth membranes, and the effect of internal concentration polarisation that is inherent of FO. It was also found that the transmission of draw solutes from the draw solution into the feed can have significant effect on FO performance.