Acid mine drainage and sewage impacted groundwater treatment by membrane distillation: Organic micropollutant and metal removal and membrane fouling.

Groundwater is the dominant source of freshwater in many countries around the globe, and the deterioration in its quality by contaminants originating from anthropogenic sources raises serious concern. In this study, a scenario where groundwater is contaminated by acid mine drainage (AMD) from mining activities and/or sewage was envisaged, and the performance of a direct contact membrane distillation (DCMD) system was investigated comprehensively for different compositions of the AMD- and sewage-impacted groundwater. Regardless of the composition, MD membrane achieved 98-100% removal of metals and bulk organics, while the removal of the selected micropollutants ranged between 80 and 100%. Effective retention of contaminants by the MD led to their accumulation over time, which affected the hydraulic performance of the MD membrane by reducing the permeate flux by 29-76%. When persulfate (PS)-mediated oxidation process was integrated with the DCMD, degradation of bulk organics (50-71%) and micropollutants (50-100%) by PS reduced their accumulation. Characterisation of the fouling layer revealed the occurrence of membrane scaling that was mainly due to the deposition of iron oxide or oxyhydroxide precipitates. For an identical composition of the AMD- and sewage-impacted groundwater, flux decline was 10% less in PS-assisted DCMD as compared to that in the standalone DCMD. However, this did not prevent the formation of iron oxide scales on MD membrane during the operation of PS-assisted DCMD. This study demonstrates the long-term performance of a standalone and PS-assisted DCMD operated in continuous-flow mode to treat AMD- and sewage-impacted groundwater for the first time.

An Osmotic Membrane Bioreactor-Membrane Distillation System for Simultaneous Wastewater Reuse and Seawater Desalination: Performance and Implications.

In this study, we demonstrate the potential of an osmotic membrane bioreactor (OMBR)-membrane distillation (MD) hybrid system for simultaneous wastewater reuse and seawater desalination. A stable OMBR water flux of approximately 6 L m-2 h-1 was achieved when using MD to regenerate the seawater draw solution. Water production by the MD process was higher than that from OMBR to desalinate additional seawater and thus account for draw solute loss due to the reverse salt flux. Amplicon sequencing on the Miseq Illumina platform evidenced bacterial acclimatization to salinity build-up in the bioreactor, though there was a reduction in the bacterial community diversity. In particular, 18 halophilic and halotolerant bacterial genera were identified with notable abundance in the bioreactor. Thus, the effective biological treatment was maintained during OMBR-MD operation. By coupling biological treatment and two high rejection membrane processes, the OMBR-MD hybrid system could effectively remove (>90%) all 30 trace organic contaminants of significant concern investigated here and produce high quality water. Nevertheless, further study is necessary to address MD membrane fouling due to the accumulation of organic matter, particularly protein- and humic-like substances, in seawater draw solution.

Continuous transformation of chiral pharmaceuticals in enzymatic membrane bioreactors for advanced wastewater treatment.

This study demonstrates continuous enantiomeric inversion and further biotransformation of chiral profens including ibuprofen, naproxen and ketoprofen by an enzymatic membrane bioreactor (EMBR) dosed with laccase. The EMBR showed non-enantioselective transformations, with high and consistent transformation of both (R)- and (S)-ibuprofen (93 ± 6%, n = 10), but lower removals of both enantiomers of naproxen (46 ± 16%, n = 10) and ketoprofen (48 ± 17%, n = 10). Enantiomeric analysis revealed a bidirectional but uneven inversion of the profens, for example 14% inversion of (R)- to (S)- compared to 4% from (S)- to (R)-naproxen. With redox-mediator addition, the enzymatic chiral inversion of both (R)- and (S)-profens remained unchanged, although the overall conversion became enantioselective; except for (S)-naproxen, the addition of redox mediator promoted the degradation of (R)-profens only.

Impact of bioplastic contamination on the mechanical recycling of conventional plastics.

Quality assurance of a recycled product is currently one of the biggest issues that the plastic recycling industry faces. The purity of the input plastic waste stream has significant influence over the quality of the recycled product. This research evaluated the impact of polylactic acid (PLA) contamination within the input waste stream of high-density polyethylene (HDPE) recycling. The ultimate tensile strength was noted to reduce by 50% when PLA contamination was at 10%. An investigation into the effect that UVA radiation (simulating solar radiation) has on HDPE contaminated with PLA was also performed to determine the long-term effect of the bioplastic contamination. After UVA treatment, the ultimate tensile strength was reported to reduce by 51% when PLA contamination was only at 2.5%. A water contact angle analysis indicated the PLA contamination increased the hydrophilic nature of the HDPE sheets, potentially creating issues if the intended use of the recycled product was to store liquids. Microscopic analysis of the HDPE sheets contaminated with PLA showed deformations, ridges, cracks, and holes appear on the surface due to the immiscibility of the two polymers that was confirmed by FTIR analysis. Colour changes were visibly noted, with UVA exposure increasing the rate of colour change. Based on the findings in this study, PLA contamination of even 1% in a HDPE waste stream would significantly reduce the quality of the recycled product.

Microplastics as an emerging contaminant of concern to our environment: a brief overview of the sources and implications.

Over the years, it has become evident that microplastics are one of the most important contaminants of concern requiring significant attention. The large abundance of microplastics that are currently in the environment poses potential toxicity risks to all organisms that are exposed to them. Microplastics have been found to affect the physiological and biological processes in marine and terrestrial organisms. As well as being a contaminant of concern in itself, microplastics also have the ability to act as vectors for other contaminants. The potential for microplastics to carry pollutants and transfer them to other organisms has been documented in the literature. Microplastics have also been linked to hosting antibiotic resistant bacteria and antibiotic resistance genes which poses a significant risk to the current health system. There has been a significant increase in research published surrounding the topic of microplastics over the last 5 years. As such, it is difficult to determine and find up to date and relevant information. This overview paper aims to provide a snapshot of the current and emerging sources of microplastics, how microplastics can act as a contaminant and have toxic effects on a range of organisms and also be a vector for a large variety of other contaminants of concern. The aim of this paper is to act as a tool for future research to reference relevant and recent literature in this field.

Antibiotic sorption onto microplastics in water: A critical review of the factors, mechanisms and implications.

Microplastics as vectors for contaminants in the environment is becoming a topic of public interest. Microplastics have been found to actively adsorb heavy metals, per-fluorinated alkyl substances (PFAS), polychlorinated biphenyls (PCBs), polyaromatic hydrocarbons (PAHs), pharmaceuticals and personal care products (PPCPs) and polybrominated diethers (PBDs) onto their surface. Particular interest in microplastics capacity to adsorb antibiotics needs further attention due to the potential role this interaction plays on antibiotic resistance. Antibiotic sorption experiments have been documented in the literature, but the data has not yet been critically reviewed. This review aims to comprehensively assess the factors that affect antibiotic sorption onto microplastics. It is recognised that the physico- chemical properties of the polymers, the antibiotic chemical properties, and the properties of the solution all play a crucial role in the antibiotic sorption capacity of microplastics. Weathering of microplastics was found to increase the antibiotic sorption capacity by up to 171%. An increase in solution salinity was found to decrease the sorption of antibiotics onto microplastics, in some instances by 100%. pH also has a substantial effect on sorption capacity, illustrating the significance of electrostatic interactions on the sorption of antibiotics onto microplastics. The need for a uniform experimental design when testing antibiotic sorption is highlighted to remove inconsistencies in the data currently presented. Current literature examines the link between antibiotic sorption and antibiotic resistance, however, further studies are still required to fully understand this emerging global crisis.

Change in the chemical, mechanical and physical properties of plastics due to UVA degradation in different water matrices: A study on the recyclability of littered plastics.

To move towards a circular society, the recyclability potential of littered plastics should be explored to provide potential value for a product that is typically destined for landfill or incineration. This study aims to understand the changes in physical, mechanical, and chemical properties of four types of plastics (polyethylene terephthalate (PET), polypropylene (PP), polycarbonate (PC) and polylactic acid (PLA) after simulated environmental degradation. Plastic samples were subjected to different water matrices (in an attempt to simulate terrestrial, ocean, and river environments) to understand the role the environment plays on plastic degradation. Significant physical, mechanical, and chemical changes were observed for the PET, PP and PLA samples. Flakes and cracks were noted during the scanning electron microscopy (SEM) analysis of PET, PP and PLA illustrating the surface degradation that had occurred. Colour scanning of the samples provided complementary information about their suitability for upcycling or downcycling. Both PET and PP had visual colour changes, making them unsuitable for upcycling purposes. PLA had a significant decrease in its tensile strength in all environmental conditions, alongside significant chemical and surface change as revealed by Fourier-transform infrared (FTIR) and SEM analysis, respectively. PC had little to no changes in its chemical, mechanical, and physical properties due to high resistance to solar (UVA) degradation in presence of salt and natural organic matter in the form of humic acid. Therefore, out of the four types of plastics tested, PC was the only plastic determined to have good upcycling potential if collected from the environment. However, PET and PP could still be recycled into lower value products (i.e., construction materials).

Identification, classification and quantification of microplastics in road dust and stormwater.

Microplastics (MP) have become a major emerging class of pollutants representing significant eco-toxicological risks for ecosystems and marine environments. The aim of this study was to identify, classify and quantify MP present in both road dust and stormwater samples. A significantly higher level of MPs within road dust samples was detected from industrial area (1130 particles/kg of dust) than from residential area (520 particles/kg of dust), while stormwater samples from industrial and residential sites yielded 26 particles/L and 17 particles/L, respectively. Fiber-like shape accounted for 53% and 74% in road dust and stormwater samples, respectively. The main polymeric materials collected for both road dust and stormwater samples were, in order of occurrence (i) low-density polyethylene, (ii) high-density polyethylene, (iii) polypropylene, (iv) polyethylene terephthalate, (v) polystyrene, (vi) polyester and (vii) poly (amide). Most of the MP had an average maximum dimension smaller than 2 mm for both road dust and stormwater samples. The results from this study demonstrates that road dust is a significant contributor to MP pollution through direct polymeric materials wear off and transfer through stormwater, which eventually will end up in open water ways and broader ecological niches.

A review of mechanisms underlying the impacts of (nano)microplastics on anaerobic digestion.

The presence of (nano)microplastics in domestic wastewater and their subsequent release to the aquatic environment via the discharge of treated sewage has raised significant concerns. Previous studies have also identified their excessive accumulation in sewage sludge. Anaerobic digestion is one of the most used sludge stabilization methods in wastewater treatment plants. Therefore, understanding the potential effects of (nano)microplastics on anaerobic digestion has been receiving increasing attention from researchers. This article provides a comprehensive review of mechanisms underlying the impacts of (nano)microplastics on anaerobic digestion. Notably, this review covers mechanisms of inhibition/enhancement of anaerobic digestion by (nano)microplastics and their potential impacts on biochemical pathways, key enzymes, functional genes, and microbial communities investigated to date. Moreover, potential environmental risks of biosolids contaminated with (nano)microplastics were highlighted. Finally, knowledge gaps and future research needs were outlined. This review will guide more standardized studies in the future, covering both fundamental and engineering aspects.

Understanding the mechanisms of trace organic contaminant removal by high retention membrane bioreactors: a critical review.

High retention membrane bioreactors (HR-MBR) combine a high retention membrane separation process such as membrane distillation, forward osmosis, or nanofiltration with a conventional activated sludge (CAS) process. Depending on the physicochemical properties of the trace organic contaminants (TrOCs) as well as the selected high retention membrane process, HR-MBR can achieve effective removal (80-99%) of a broad spectrum of TrOCs. An in-depth assessment of the available literature on HR-MBR performance suggests that compared to CAS and conventional MBRs (using micro- or ultra-filtration membrane), aqueous phase removal of TrOCs in HR-MBR is significantly better. Conceptually, longer retention time may significantly improve TrOC biodegradation, but there are insufficient data in the literature to evaluate the extent of TrOC biodegradation improvement by HR-MBR. The accumulation of hardly biodegradable TrOCs within the bioreactor of an HR-MBR system may complicate further treatment and beneficial reuse of sludge. In addition to TrOCs, accumulation of salts gradually increases the salinity in bioreactor and can adversely affect microbial activities. Strategies to mitigate these limitations are discussed. A qualitative framework is proposed to predict the contribution of the different key mechanisms of TrOC removal (i.e., membrane retention, biodegradation, and sorption) in HR-MBR.

An anaerobic membrane bioreactor - membrane distillation hybrid system for energy recovery and water reuse: Removal performance of organic carbon, nutrients, and trace organic contaminants.

In this study, a direct contact membrane distillation (MD) unit was integrated with an anaerobic membrane bioreactor (AnMBR) to simultaneously recover energy and produce high quality water for reuse from wastewater. Results show that AnMBR could produce 0.3-0.5L/g CODadded biogas with a stable methane content of approximately 65%. By integrating MD with AnMBR, bulk organic matter and phosphate were almost completely removed. The removal of the 26 selected trace organic contaminants by AnMBR was compound specific, but the MD process could complement AnMBR removal, leading to an overall efficiency from 76% to complete removal by the integrated system. The results also show that, due to complete retention, organic matter (such as humic-like and protein-like substances) and inorganic salts accumulated in the MD feed solution and therefore resulted in significant fouling of the MD unit. As a result, the water flux of the MD process decreased continuously. Nevertheless, membrane pore wetting was not observed throughout the operation.

Assessing the integration of forward osmosis and anaerobic digestion for simultaneous wastewater treatment and resource recovery.

This study assessed the performance and key challenges associated with the integration of forward osmosis (FO) and anaerobic digestion for wastewater treatment and resource recovery. Using a thin film composite polyamide FO membrane, maximising the pre-concentration factor (i.e. system water recovery) resulted in the enrichment of organics and salinity in wastewater. Biomethane potential evaluation indicated that methane production increased correspondingly with the FO pre-concentration factor due to the organic retention in the feed solution. At 90% water recovery, about 10% more methane was produced when using NaOAc compared with NaCl because of the contribution of biodegradable reverse NaOAc flux. No negative impact on anaerobic digestion was observed when wastewater was pre-concentrated ten-fold (90% water recovery) for both draw solutes. Interestingly, the unit cost of methane production using NaOAc was slightly lower than NaCl due to the lower reverse solute flux of NaOAc, although NaCl is a much cheaper chemical.

Effect of hydraulic retention time on the performance of a hybrid moving bed biofilm reactor-membrane bioreactor system for micropollutants removal from municipal wastewater.

This study evaluated micropollutants removal and membrane fouling behaviour of a hybrid moving bed biofilm reactor-membrane bioreactor (MBBR-MBR) system at four different hydraulic retention times (HRTs) (24, 18, 12 and 6h). The results revealed that HRT of 18h was the optimal condition regarding the removal of most selected micropollutants. As the primary removal mechanism in the hybrid system was biodegradation, the attached growth pattern was desirable for enriching slow growing bacteria and developing a diversity of biocoenosis. Thus, the efficient removal of micropollutants was obtained. In terms of membrane fouling propensity analysis, a longer HRT (e.g. HRTs of 24 and 18h) could significantly mitigate membrane fouling when compared with the shortest HRT of 6h. Hence, enhanced system performance could be achieved when the MBBR-MBR system was operated at HRT of 18h.

Impact of simultaneous retention of micropollutants and laccase on micropollutant degradation in enzymatic membrane bioreactor.

This study systematically compares the performance of ultrafiltration (UF) and nanofiltration (NF) based enzymatic membrane bioreactors (EMBRs) for the degradation of five micropollutants, namely atrazine, carbamazepine, sulfamethoxazole, diclofenac and oxybenzone to elucidate the impact of effective membrane retention of micropollutants on their degradation. Based on the permeate quality, NF-EMBR achieved 92-99.9% micropollutant removal (i.e., biodegradation + membrane retention), while the removal of these micropollutants by UF-EMBR varied from 20 to 85%. Mass balance analysis revealed that micropollutant degradation was improved by 15-30% in NF-EMBR as compared to UF-EMBR, which could be attributed to the prolonged contact time between laccase and micropollutants following their effective retention by the NF membrane. A small decline in permeate flux was observed during EMBR operation. However, the flux could be recovered by flushing the membrane with permeate.

Effects of sulphur on the performance of an anaerobic membrane bioreactor: Biological stability, trace organic contaminant removal, and membrane fouling.

This study investigated the impact of sulphur content on the performance of an anaerobic membrane bioreactor (AnMBR) with an emphasis on the biological stability, contaminant removal, and membrane fouling. Removal of 38 trace organic contaminants (TrOCs) that are ubiquitously present in municipal wastewater by AnMBR was evaluated. Results show that basic biological performance of AnMBR regarding biomass growth and the removal of chemical oxygen demand (COD) was not affected by sulphur addition when the influent COD/SO42- ratio was maintained higher than 10. Nevertheless, the content of hydrogen sulphate in the produced biogas increased significantly and membrane fouling was exacerbated with sulphur addition. Moreover, the increase in sulphur content considerably affected the removal of some hydrophilic TrOCs and their residuals in the sludge phase during AnMBR operation. By contrast, no significant impact on the removal of hydrophobic TrOCs was noted with sulphur addition to AnMBR.

Biocatalytic degradation of pharmaceuticals, personal care products, industrial chemicals, steroid hormones and pesticides in a membrane distillation-enzymatic bioreactor.

Laccase-catalyzed degradation of a broad spectrum of trace organic contaminants (TrOCs) by a membrane distillation (MD)-enzymatic membrane bioreactor (EMBR) was investigated. The MD component effectively retained TrOCs (94-99%) in the EMBR, facilitating their continuous biocatalytic degradation. Notably, the extent of TrOC degradation was strongly influenced by their molecular properties. A significant degradation (above 90%) of TrOCs containing strong electron donating functional groups (e.g., hydroxyl and amine groups) was achieved, while a moderate removal was observed for TrOCs containing electron withdrawing functional groups (e.g., amide and halogen groups). Separate addition of two redox-mediators, namely syringaldehyde and violuric acid, further improved TrOC degradation by laccase. However, a mixture of both showed a reduced performance for a few pharmaceuticals such as primidone, carbamazepine and ibuprofen. Mediator addition increased the toxicity of the media in the enzymatic bioreactor, but the membrane permeate (i.e., final effluent) was non-toxic, suggesting an added advantage of coupling MD with EMBR.

Osmotic versus conventional membrane bioreactors integrated with reverse osmosis for water reuse: Biological stability, membrane fouling, and contaminant removal.

This study systematically compares the performance of osmotic membrane bioreactor - reverse osmosis (OMBR-RO) and conventional membrane bioreactor - reverse osmosis (MBR-RO) for advanced wastewater treatment and water reuse. Both systems achieved effective removal of bulk organic matter and nutrients, and almost complete removal of all 31 trace organic contaminants investigated. They both could produce high quality water suitable for recycling applications. During OMBR-RO operation, salinity build-up in the bioreactor reduced the water flux and negatively impacted the system biological treatment by altering biomass characteristics and microbial community structure. In addition, the elevated salinity also increased soluble microbial products and extracellular polymeric substances in the mixed liquor, which induced fouling of the forward osmosis (FO) membrane. Nevertheless, microbial analysis indicated that salinity stress resulted in the development of halotolerant bacteria, consequently sustaining biodegradation in the OMBR system. By contrast, biological performance was relatively stable throughout conventional MBR-RO operation. Compared to conventional MBR-RO, the FO process effectively prevented foulants from permeating into the draw solution, thereby significantly reducing fouling of the downstream RO membrane in OMBR-RO operation. Accumulation of organic matter, including humic- and protein-like substances, as well as inorganic salts in the MBR effluent resulted in severe RO membrane fouling in conventional MBR-RO operation.

New and practical mathematical model of membrane fouling in an aerobic submerged membrane bioreactor.

This study aimed to develop a practical semi-empirical mathematical model of membrane fouling that accounts for cake formation on the membrane and its pore blocking as the major processes of membrane fouling. In the developed model, the concentration of mixed liquor suspended solid is used as a lumped parameter to describe the formation of cake layer including the biofilm. The new model considers the combined effect of aeration and backwash on the foulants' detachment from the membrane. New exponential coefficients are also included in the model to describe the exponential increase of transmembrane pressure that typically occurs after the initial stage of an MBR operation. The model was validated using experimental data obtained from a lab-scale aerobic sponge-submerged membrane bioreactor (MBR), and the simulation of the model agreed well with the experimental findings.

Factors governing the pre-concentration of wastewater using forward osmosis for subsequent resource recovery.

This study demonstrated a technique using forward osmosis (FO) to pre-concentrate the organic matter in raw wastewater, thereby transforming low strength wastewater into an anaerobically digestible solution. The chemical oxygen demand (COD) of raw wastewater was concentrated up to approximately eightfold at a water recovery of 90%. Thus, even low strength wastewater could be pre-concentrated by FO to the range suitable for biogas production via anaerobic treatment. Excessive salinity accumulation in pre-concentrated wastewater was successfully mitigated by adopting ionic organic draw solutes, namely, sodium acetate, and EDTA-2Na. These two draw solutes are also expected to benefit the digestibility of the pre-concentrated wastewater compared to the commonly used draw solute sodium chloride. Significant membrane fouling was observed when operating at 90% water recovery using raw wastewater. Nevertheless, membrane fouling was reversible and was effectively controlled by optimising the hydrodynamic conditions of the cross-flow FO system.

Effects of salinity build-up on the performance of an anaerobic membrane bioreactor regarding basic water quality parameters and removal of trace organic contaminants.

The effects of elevated inorganic salt concentration on anaerobic membrane bioreactor (AnMBR) treatment regarding basic biological performance and trace organic contaminant (TrOC) removal were investigated. A set of 33 TrOCs were selected to represent pharmaceuticals, steroids, and pesticides in municipal wastewater. Results show potential adverse effects of increase in the bioreactor salinity to 15g/L (as NaCl) on the performance of AnMBR with respect to chemical oxygen demand removal, biogas production, and the removal of most hydrophilic TrOCs. Furthermore, a decrease in biomass production was observed as salinity in the bioreactor increased. The removal of most hydrophobic TrOCs was high and was not significantly affected by salinity build-up in the bioreactor. The accumulation of a few persistent TrOCs in the sludge phase was observed, but such accumulation did not vary significantly as salinity in the bioreactor increased.