•PFAS occurrence information is not available for most developing countries.•Monitoring is required for ultra-short chain and new generation replacement PFAS.•Majority of studies report higher PFAS ...concentrations in effluents than influents.•Biodegradation transforms PFAS precursors to PFAA at a secondary stage.•Adsorption, electrochemical, and filtration are the most studied PFAS treatments.
Poly- and perfluoroalkyl substances (PFAS) comprise more than 4,000 anthropogenically manufactured compounds with widescale consumer and industrial applications. This critical review compiles the latest information on the worldwide distribution of PFAS and evaluates their fate in wastewater treatment plants (WWTPs). A large proportion (>30%) of monitoring studies in WWTPs were conducted in China, followed by Europe (30%) and North America (16%), whereas information is generally lacking for other parts of the world, including most of the developing countries. Short and long-chain perfluoroalkyl acids (PFAAs) were widely detected in both the influents (up to 1,000 ng/L) and effluents (15 to >1,500 ng/L) of WWTPs. To date, limited data is available regarding levels of PFAS precursors and ultra-short chain PFAS in WWTPs. Most WWTPs exhibited low removal efficiencies for PFAS, and many studies reported an increase in the levels of PFAAs after wastewater treatment. The analysis of the fate of various classes of PFAS at different wastewater treatment stages (aerobic and/aerobic biodegradation, photodegradation, and chemical degradation) revealed biodegradation as the primary mechanism responsible for the transformation of PFAS precursors to PFAAs in WWTPs. Remediation studies at full scale and laboratory scale suggest advanced processes such as adsorption using ion exchange resins, electrochemical degradation, and nanofiltration are more effective in removing PFAS (~95–100%) than conventional processes. However, the applicability of such treatments for real-world WWTPs faces significant challenges due to the scaling-up requirements, mass-transfer limitations, and management of treatment by-products and wastes. Combining more than one technique for effective removal of PFAS, while addressing limitations of the individual treatments, could be beneficial. Considering environmental concentrations of PFAS, cost-effectiveness, and ease of operation, nanofiltration followed by adsorption using wood-derived biochar and/or activated carbons could be a viable option if introduced to conventional treatment systems. However, the large-scale applicability of the same needs to be further verified.
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The occurrence and removal of thirty representative pharmaceutical and personal care products (PPCPs) and endocrine disrupting chemicals (EDCs) in an urban drinking water treatment plant (DWTP) were ...investigated for a period of one year to evaluate current system's treatment efficacy and assess occurrence of PPCPs and EDCs in finished drinking water. Results showed that the average total PPCPs and EDCs concentration in the surface water source was around 360 ng/L (median concentration = 340 ng/L) with 57% coefficient of variation (CV). The median concentrations of most of the individual PPCPs and EDCs in the surface water were below 15 ng/L except for N,N-diethyltoluamide (DEET) and nonylphenol, which were at 122 and 83 ng/L, respectively. The compounds DEET, nonylphenol, ibuprofen, triclosan, atrazine, tris(2-chloroethyl)-phosphate (TCEP), bisphenol-A, and caffeine (in the order of decreasing median concentration) were among twenty compounds detected at least once in the surface water, while all of the above detected compounds, except two, were also detected in the finished drinking water. The average total PPCPs and EDCs concentration in the finished drinking water was around 98 ng/L (median concentration = 96 ng/L) with 66% CV. The median concentrations of most detected PPCPs and EDCs in drinking water were below 5 ng/L except for DEET and nonylphenol, which were at 12 and 20 ng/L, respectively. There was a strong correlation (r = 0.97) between PPCPs and EDCs' concentrations in the source water and in the drinking water over the one-year study period when data points from two sampling events with unusual removals were excluded. Individual water treatment unit processes showed greater temporal variations of PPCPs and EDCs removal efficiencies than the overall treatment processes. The removal efficiencies also varied greatly among different PPCPs and EDCs. The average removal for total PPCPs and EDCs was 76 ± 18% at the DWTP, with ozonation showing the highest removal efficiency. Based on the similar occurrence and removal trends observed as that of total PPCPs and EDCs in this study, DEET and nonylphenol can be considered as potential indicator compounds for predicting the occurrence and removal of total PPCPs and EDCs in surface water. No strong correlations could be found between total PPCPs and EDCs removal and the removal of suspended solids, turbidity, or organic carbon.
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•30 PPCPs and EDCs were monitored at an urban drinking water treatment plant for one year.•Average total concentration of PPCPs and EDCs was at 360 and 98 ng/L in source water and finished drinking water, respectively.•Significant seasonal variations existed in concentrations and removal efficiencies for PPCPs and EDCs.•Overall, ozonation showed the highest removal efficiency for PPCPs and EDCs.•DEET and nonylphenol, detected at the highest concentrations, could be considered indicators for PPCPs and EDCs.
The objective of this study was to study the occurrence, fate, and seasonal variations of pharmaceuticals at two urban wastewater treatment plants (WWTPs) in India and compare the results with a ...similar study conducted in the United States. This is the first study of its kind in comparing occurrence and fate of pharmaceuticals in wastewater of two different countries with the same methodology and analytical techniques. Twelve most relevant pharmaceuticals were selected for seasonal monitoring at two Indian WWTPs based on the comprehensive survey and through literature review. The yearly average influent concentrations of total pharmaceuticals were found to be 537 ± 5 μg/L at WWTP-1 and 353 ± 9 μg/L at WWTP-2. WWTP-2 exhibited comparatively higher removal efficiency of total pharmaceuticals (85% versus 59%, excluding monsoon season), possibly due to the cyclic activated sludge technology followed by chlorination employed at WWTP-2. Comparison with a similar study conducted in the United States revealed that concentration of most of the pharmaceuticals detected in the U.S. WWTPs were, on an average, more than 50% lower. U.S. WWTPs also exhibited 10–30% higher removal efficiencies for total pharmaceuticals. Our study results show that preliminary treatment and biological treatment alone are not adequate for complete removal of pharmaceuticals and polishing step and tertiary treatment is a necessity if higher removal of pharmaceuticals is desired in Indian WWTPs. Information obtained from this study will not only aid the local utilities but will also benefit understanding of global trends in usage of pharmaceuticals and their distribution in the environment.
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•Seasonal occurrence and fate of 12 pharmaceuticals at two Indian WWTPs.•Average influent PPCPs detected at 537 μg/L and 353 μg/L at Indian WWTPs.•85% PPCPs removal in WWTP-2 versus 59% in WWTP-1.•PPCPs concentrations in U.S. WWTPs were more than 50% lower.•U.S. WWTPs exhibited 10–30% higher PPCPs removal efficiencies.
Seasonal variations in the concentrations and fate of 20 selected pharmaceuticals and personal care products (PPCPs) were investigated over one year in a wastewater treatment plant in New Zealand, ...which relies on a membrane bioreactor (MBR) and Bardenpho as parallel processes for its secondary treatment. Results showed that all of the monitored PPCPs were detected in the wastewater influent. Nonsteroidal anti-inflammatory drugs (NSAIDS) and caffeine were predominant in the influent, whereas in the effluent, β-blockers and benzotriazole were present at significant concentrations. Total PPCPs' concentration in the influent was found to be 130 μg/L. Average removal efficiency was found to be ≥ 99% for acetaminophen, caffeine, TCEP, naproxen, and ibuprofen, whereas <50% of trimethoprim, metoprolol, and benzotriazole were removed. Contrary to the existing literature, no significant differences were found in the removal of PPCPs through MBR and Bardenpho processes, hinting that optimally operated Bardenpho can be equally effective in the removal of emerging contaminants as MBR. The occurrence and removal efficiencies of PPCPs were found to exhibit significant seasonal variations, with the highest influent concentrations of PPCPs reported in autumn and winter. Heavy rainfall had an insignificant impact on PPCPs' removal efficiencies although it resulted in much-diluted concentrations of PPCPs in the influent. Spearman's correlation analysis showed significant correlations between PPCPs' mass loads in the influent, wastewater quality parameters, and environmental factors. It was also found that, except sulfamethoxazole, ecotoxicity risks were minimal for the rest of the monitored PPCPs in wastewater effluent.
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•First inter-seasonal PPCPs' study in New Zealand's wastewater treatment plant.•Significant mass load of antibiotics discharged to the environment.•Bardenpho and MBR showed comparable removal efficiencies.•Correlations between PPCPs' occurrence, removal and wastewater quality parameters.
The extensive usage of high-density polyethylene (HDPE) materials in marine environments raises concerns about their potential contribution to plastic pollution. Various factors contribute to the ...degradation of HDPE in marine environments, including UV radiation, seawater hydrolysis, biodegradation, and mechanical stress. Despite their supposed long lifespans, there is still a lack of understanding about the long-term degradation mechanisms that cause weathering of seawater-exposed HDPE products. In this research, the impact of UV radiation on the degradation of HDPE pile sleeves was studied in natural as well as laboratory settings to isolate the UV effect. After nine years of exposure to the marine environment in natural settings, the HDPE pile sleeves exhibited an increase in oxygen-containing surface functional groups and more morphological changes compared to accelerated UVB irradiation in the laboratory. This indicated that combined non-UV mechanisms may play a major role in HDPE degradation than UV irradiation alone. However, UVB irradiation was found to release dissolved organic carbon and total dissolved nitrogen from HDPE pile sleeves, reaching levels of up to 15 mg/L and 2 mg/L, respectively. Our findings underscore the significance of taking into account both UV and non-UV degradation mechanisms when evaluating the role of HDPE in contributing to marine plastic pollution.
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•Commercially marketed HDPE sleeves offered excellent UV protection.•Long-term HDPE degradation revealed the overlooked role of non-UV processes.•Surface oxidation of HDPE was higher in natural settings than in the laboratory.•Up to 280 mg TDN/kg HDPE leached under accelerated UVB irradiation.•Up to 2285 mg DOC/kg HDPE leached under accelerated UVB irradiation.
Conventional water resources in many regions are insufficient to meet the water needs of growing populations, thus reuse is gaining acceptance as a method of water supply augmentation. Recent ...advancements in membrane technology have allowed for the reclamation of municipal wastewater for the production of drinking water, i.e., potable reuse. Although public perception can be a challenge, potable reuse is often the least energy-intensive method of providing additional drinking water to water stressed regions. A variety of membranes have been developed that can remove water contaminants ranging from particles and pathogens to dissolved organic compounds and salts. Typically, potable reuse treatment plants use polymeric membranes for microfiltration or ultrafiltration in conjunction with reverse osmosis and, in some cases, nanofiltration. Membrane properties, including pore size, wettability, surface charge, roughness, thermal resistance, chemical stability, permeability, thickness and mechanical strength, vary between membranes and applications. Advancements in membrane technology including new membrane materials, coatings, and manufacturing methods, as well as emerging membrane processes such as membrane bioreactors, electrodialysis, and forward osmosis have been developed to improve selectivity, energy consumption, fouling resistance, and/or capital cost. The purpose of this review is to provide a comprehensive summary of the role of polymeric membranes and process components in the treatment of wastewater to potable water quality and to highlight recent advancements and needs in separation processes. Beyond membranes themselves, this review covers the background and history of potable reuse, and commonly used potable reuse process chains, pretreatment steps, and advanced oxidation processes. Key trends in membrane technology include novel configurations, materials, and fouling prevention techniques. Challenges still facing membrane-based potable reuse applications, including chemical and biological contaminant removal, membrane fouling, and public perception, are highlighted as areas in need of further research and development.
N-Nitrosamines, well-known human carcinogens, are widely considered to be formed through the disinfection of waters containing compounds with amine moieties. The formation mechanisms of nitrosamines ...during the disinfection of drinking water and wastewater have been previously reviewed in the literature. However, no study to date has reviewed the effects of inorganic ions on nitrosamines formation during disinfection. Inorganic ions are ubiquitous in the environment and are present at significant concentrations in water and wastewater. Their presence influences aqueous nitrosamines formation, depending on the type, concentration, and environmental conditions. In this review, we have critically reviewed nitrosamines' precursors and occurrence, disinfection processes associated with nitrosamines' formation/destruction, and the impact of inorganic ions on the formation or removal of nitrosamines during disinfection of water and wastewater. The disinfectants reviewed in the study were chlorine, chloramine, chlorine dioxide, ozone, and radicals generated through advanced oxidation processes (AOPs). N-Nitrosodimethylamine formation pathways, in the presence and absence of inorganic ions, were also reviewed to summarize our current understanding. Although chloramination has been associated with the formation of nitrosamines, many ozonation studies have also shown significant levels of nitrosamines formation. Pre-oxidation and AOPs have been reported as the most promising mitigation strategies for controlling nitrosamines formation, requiring prolonged exposure of precursors for effective mineralization.
•Overlooked contribution of PBMs towards the DBP formation was critically reviewed.•Elastomers, tire waste, polyelectrolytes, and MPs serve as potent DBP precursors.•Leached DOC and dissolved ...nitrogen from PBMs play a key role in DBP formation.•DBPs formation potential of polyelectrolytes was found as high as ∼2 mg/L.•DBPs formation potential of different microplastics ranged from 1.9 to 15,990 µg/L.
Disinfection by-products (DBPs) are formed through the disinfection of water containing precursors such as natural organic matter or anthropogenic compounds (e.g., pharmaceuticals and pesticides). Due to the ever increasing use of plastics, elastomers, and other polymers in our daily lives, polymer-based materials (PBMs) are detected more frequently and at higher concentrations in water and wastewater. The present review provides a comprehensive and systematic analysis of the contribution of PBMs - including elastomers, tire waste, polyelectrolytes, and microplastics - as precursors of DBPs in water and wastewater. Literature shows that the presence of PBMs can lead to the leaching of dissolved organic matter (DOM) and subsequent formation of DBPs upon disinfection in aqueous media. The quantity and type of DBPs formed strongly depends on the type of polymer, its concentration, its age, water salinity, and disinfection conditions such as oxidant dosage, pH, temperature, and contact time. DOM leaching from elastomers and tire waste was shown to form N-nitrosodimethylamine up to concerning levels of 930 ng/L and 466,715 ng/L, respectively upon chemical disinfection under laboratory conditions. Polyelectrolytes can also react with chemical disinfectants to form toxic DBPs. Recent findings indicate trihalomethanes formation potential of plastics can be as high as 15,990 µg/L based on the maximum formation potential under extreme conditions. Our analysis highlights an overlooked contribution of DOM leaching from PBMs as DBP precursors during disinfection of water and wastewater. Further studies need to be conducted to ascertain the extent of this contribution in real water and wastewater treatment plants.
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Information on the occurrence of PFAS in aquatic matrices of countries with no PFAS manufacturing, e.g., New Zealand, is limited. Also, the fingerprint of PFAS along an urban water cycle, following ...water path from wastewater treatment plant (WWTP) effluent to treated drinking water has not been widely assessed. Hence, 38 long-, short-, ultrashort-chain PFAS and fluorinated alternatives (including precursors) were monitored in this study by collecting composite samples from two urban WWTPs of New Zealand and grab samples from the water bodies receiving the WWTPs’ effluents and a drinking water treatment plant, whose source water received the effluent of one of the studied WWTPs. ∑PFAS at concentrations 0.1 – 13 ng/L were detected in all wastewater samples, including influents and different treatment stages of the two WWTPs (WW1 and WW2). The fate of most PFAS was similar in the two WWTPs, despite large differences in WWTPs’ PFAS loads in the influents, serving populations (1.6 vs 0.16 million), total capacities (300 vs 54 million liters per day), and designs (aerobic and anoxic secondary treatment vs aerobic only). The fate of PFAS in WWTPs appeared to be driven by a range of processes. For instance, a simultaneous increase (41.6%) in short-chain perfluorohexanoic acid (PFHxA) concentrations and decrease (49.7%) in precursor 6:2 fluorotelomer sulfonate (6:2 FTS) concentrations after secondary biological treatment suggested possible transformation of 6:2 FTS into PFHxA during the treatment. In contrast, the reason behind an average decrease of 35% in ultrashort-chain perfluoropropionic acid (PFPrA) concentrations after treatment was unclear, and further studies are recommended. The concentrations of a linear isomer of long-chain perfluorosulfonic acid (PFOS-L) decreased (48%) in the effluent, possibly due to its partitioning to sludge. Although the concentrations of PFAS in coastal waters suggested that the WW1 effluent is a potential source of PFAS, earlier dispersion model and no detection of PFAS in the receiving waters of WW2 implied that other sources, such as septic systems, peripheral industries, and the airport, could also be contributing to PFAS in coastal waters. The source of ultrashort-chain PFPrA (5.5 ng/L) detected in the treated drinking water produced from that river was unclear. The monitoring results confirm incomplete removal of PFAS in WWTPs, indicate a possible transformation of unknown precursors present in wastewater into short-chain perfluoroalkylcarboxylic acids (PFCAs) during biological treatment, and reveal a possible accumulation of perfluoroalkylsulfonic acids (PFSAs) in the sludge, overall suggesting the circulation of PFAS in urban water systems.
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•Long-, short- and ultrashort-chain PFAS detected in two urban WWTPs of New Zealand.•Ultrashort-chain PFPrA detected in treated drinking water.•A combination of sources contributed to PFAS detected in coastal waters.•6:2 FTS could transform to short-chain PFHxA during secondary biological treatment.•Partitioning of long-chain PFOS to sludge could explain its presence in biosolids.
Elucidation of mechanistic insight into the interaction of carbon materials' physicochemical surface properties and ammonium (NH4+) adsorption in aqueous media was made by conducting a systematic ...study using a wide range of carbon materials. Three types of biochars (rice husk, poultry litter, and enhanced poultry litter) and activated carbons (fresh and aged coconut shell-based and charcoal-based) were used for investigating the NH4+ adsorption mechanism. Poultry litter biochar, with lowest surface area (3 m2 g−1) and largest pore diameter (29 nm), showed the highest NH4+ adsorption capacity (0.34 mg NH4+g−1), while charcoal-based activated carbon, with the highest surface area (1133 m2 g−1) and small pore diameter (6 nm), had the least NH4+ adsorption capacity (0.09 mg NH4+g−1). The value of Freundlich isotherm constant ‘n’ was >1 for all tested carbon materials indicating chemisorption as the dominant sorption mechanism. Aging of the carbon surface resulted in 30% increase in NH4+ retention. Surface chemical properties that most influenced NH4+ chemisorption on to carbon materials were found to be acidic surface functional groups (ASFGs), elemental composition, ash content, and pH. The optimal conditions for NH4+ adsorption, regardless of type and source of carbon materials, were solution pH of 8, a high amount of ash content, and carboxyl, carbonyl, and phenolic functional groups. Evaluation of CEC and ASFGs indicated that CEC and ASFGs are not equivalent terms. Through this study, conducted on carbon adsorbents derived from different sources, with different surface physical and chemical properties, we established that ASFGs, and not CEC, play a critical role in ammonium chemisorption on carbon materials. The study showed that low cost and eco-friendly biochars, with optimal surface chemistry, can replace expensive activated carbons for NH4+ remediation in aqueous media.
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•Chemisorption is a dominant adsorption mechanism of NH4+ on the carbon surface.•Carboxyl, carbonyl, and phenolic surface functional groups dominate NH4+ adsorption.•Cation exchange capacity and acidic surface functional groups are not equivalent.•Biochars with optimal surface chemistry adsorb NH4+ better than activated carbon.
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