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Swimming pools adopt chlorination to ensure microbial safety. Giardia has attracted attention in swimming pool water because of its occurrence, pathogenicity, and chlorine resistance. To control Giardia concentrations in pool water and reduce the microbial risk, higher chlorine doses are required during disinfection. Unfortunately, this process produces carcinogenic disinfection byproducts that increase the risk of chemical exposure. Therefore, quantitatively evaluating the comparative microbial vs. chemical exposure risks that stem from chlorination inactivation of Giardia in swimming pool water is an issue that demands attention. We simulated an indoor swimming pool disinfection scenario that followed common real-world disinfection practices. A quantitative microbial risk assessment coupled with a chemical exposure risk assessment was employed to compare the Giardia microbial exposure risk (MER) and the trihalomethane chemical exposure risk (CER) to humans. The results demonstrated a 22% decrease in MER- and CER-induced health exposure risk, from 8.45E-5 at 8:00 to 6.60E-5 at 19:00. Both the MER and CER decreased gradually, dropping to 3.26E-5 and 3.35E-5 at 19:00, respectively. However, the CER exceeded the MER after 18:30 and became the dominant factor affecting the total exposure risk. Past the 18 hr mark, the contribution of trihalomethane CER far exceeded the risk aversion from microbial inactivation, leading to a net increase in total exposure risk despite the declining MER. Swimmers may consider swimming after 19:00, when the total exposure risk is the lowest. Lowering water temperature and/or pH were identified as the most sensitive factors to minimize the overall health exposure risk.

Quantification of regulated and emerging disinfection byproducts (DBPs) in swimming pool water, as well as the assessment of their lifetime health risk are limited in China. In this study, the occurrence of regulated DBPs (e.g., trihalomethanes, haloacetic acids) and emerging DBPs (e.g., haloacetonitriles, haloacetaldehydes) in indoor swimming pool water and the corresponding source water at a city in Eastern China were determined. The concentrations of DBPs in swimming pool water were 1-2 orders of magnitude higher than that in source water. Lifetime cancer and non-cancer risks of DBPs stemming from swimming pool water were also estimated. Inhalation and dermal exposure were the most significant exposure routes related to swimming pool DBP cancer and non-cancer risks. For the first time, buccal and aural exposure were considered, and were proven to be important routes of DBP exposure (accounting for 17.9%-38.9% of total risk). The cancer risks of DBPs for all swimmers were higher than 10

Reuse of water requires the removal of contaminants to ensure human health. We report the relative estrogenic activity (REA) of reuse treatment design scenarios for water, wastewaters, and processed wastewaters before and after pilot-scale treatment systems tested at select military facilities. The comparative relationships between REA, several composite toxicological endpoints, and spectroscopic indicators were evaluated for different reuse treatment trains. Four treatment processes including conventional and advanced treatments reduced the estrogenicity by at least 33%. Biologically based methods reduced estrogenicity to below detection levels. Conventional treatment scenarios led to significantly less reduction of adverse biological endpoints compared to the advanced treatment scenarios. Incorporating the anaerobic membrane bioreactor reduced more endpoints with higher reduction percentages compared to the sequencing batch reactor design. Membrane technology and advanced oxidation generated reductions across all biological endpoints, from 65% (genotoxicity) to 100% (estrogenicity). The design scenarios featuring a low-cutoff mechanical screen filter, intermittent activated carbon biofilter, and membrane filtration achieved the highest percent reduction and produced water with the lowest negative biological endpoints. Spectroscopic indicators demonstrated case-specific relationships with estrogenicity and toxicity. Estrogenicity consistently correlated with cytotoxicity and thiol reactivity, indicating the potential for preliminary estrogenicity screening using thiol reactivity.

Recycling wastewater from animal production for fertilizers using anaerobic digestion (AD) is a common method to recover the nutrients in the digestate. However, the digestate toxicity is not well understood because AD is mainly designed for chemical oxygen demand reduction. This study determined the toxicity during AD and the controlling factors with the goal to improve digestate safety during farmer handling to reuse the nutrients. Thermophilic and mesophilic AD of two swine wastewater sources were studied. Mammalian cell cytotoxicity revealed that the effluent after thermophilic digestion was at least 69% more toxic than the mesophilic effluent, owing to higher ammonia and total organic carbon in the former. Ammonia accounted for55% total cytotoxicity, and the organics of the thermophilic digestate were twice more toxic than those in the mesophilic digestate. Despite less toxicity contribution than the ammonia, the organics did demonstrate significant adverse effects on the thiol-mediated cellular protection mechanism. For swine wastewater nutrient recovery, converting ammonia to less toxic nitrogen forms could lower the toxic hazard of the AD digestate. With much less ammonia, the organics would be the remaining decisive factor for toxicity, which is favorably reduced using thermophilic AD over mesophilic. If the ammonia is not reduced, mesophilic AD would generate a less toxic digestate.

Decentralized direct potable reuse systems present new opportunities and potential risks for resilient and sustainable facilities of the future. This study explored the use of advanced cell-based composite toxicity methods to augment the assessment of known and unknown chemicals in waters from decentralized direct potable reuse systems. The decentralized reuse systems were equipped with newly-developed low energy membranes and advanced oxidation technologies for the control of the full spectrum of contaminants found in wastewater effluent. The feed and product waters from these systems were tested for conventional chemical contaminants, personal care and pharmaceutical products, composite cytotoxicity and composite genotoxicity. The composite toxicity assays confirmed the high degree of purification in the decentralized potable reuse systems and responded accordingly when known contaminants were detected at levels approaching or exceeding regulatory limits. The composite toxicity assays identified potential risks for water samples that would not be considered contaminated or a risk to health based on conventional contaminant monitoring. Unknown disinfection byproducts appeared to be the causal factors due to increases in cytotoxicity that occurred during the disinfection step. It is recommended that composite toxicity assays be considered to augment validation and optimization of direct potable reuse systems to minimize potential health risks associated with the additive effects of known and unknown contaminants.

In China, urea degradants are often used in combination with chlorine in swimming pool water to remove urea. Here we report the first study about the impacts of urea degradants on urea degradation, disinfection byproduct (DBP) formation and estimated DBP-associated cytotoxicity and genotoxicity. Firstly, four groups of typical DBPs from six real indoor swimming pools were analyzed. The concentration of DBPs in swimming pool waters was about 1-2 orders of magnitude higher than that source tap water. Notably, a rapid increase in DBPs was observed after urea degradant treatment. Simulated processes of urea removal using three commonly used urea degradants were therefore conducted in laboratory. Neither urea degradant nor chlorine alone removed urea effectively within 48 h. When applied in combination, urea degradant with sufficient chlorine rapidly removed urea by 100% within 3 h, and anti-chlorourea oligomer in urea degradants was the main contributor. Meanwhile, a remarkable increase in DBPs, especially brominated DBPs, was observed due to bromide introduction by urea degradants. For this reason, bromine incorporation factor (BIF) of DBPs dramatically increased. For instance, the BIF of dihaloacetic acids increased by 2665%-4025% after applying three urea degradants. As the highly toxic brominated DBPs were generated, attention should be paid into the potential DBP-related health risks from the use of urea degradants together with chlorine.

Efforts to remove highly toxic haloacetonitriles (HANs) is an important step to reduce health risks associated with disinfection by product exposure. Zero valent iron (ZVI) is a versatile material, whose reductant, sorbent and coagulant role has been well understood. However, their catalytic role is less known. In this study, the degradation and transformation of HANs in ZVI system were investigated. Significant decreases of the four HANs in ZVI system were observed, and haloacetamides and haloacetic acids (hydrolysis products of HANs) were the dominant transformation products of HANs. However dehalogenated HANs, Fe (II) and Fe (III) were rarely detected after reaction, indicating that the ZVI acted as a catalyst to promote the hydrolysis of HANs, rather than other previously reported causes (dehalogenation or redox reaction). The HAN degradation rates were dramatically affected by the initial pH, ZVI doses and initial HAN concentration. Kinetic analysis indicated that HAN removal was enhanced with the increase of initial pH (5-9), ZVI doses (1-10 g/L), and initial HAN concentration (25-200 μg/L). ZVI induced the transformation of HANs to haloacetamides, haloacetic acids and other de-halogenated compounds, which reduced the cytotoxicity and genotoxicity by 88% and 85%, respectively. This study helped to understand the fate of HAN during the transmission in cast iron pipes, and provided a theoretical foundation for future HAN control and monitoring efforts.

As the coronavirus disease 2019 continues to spread globally, its culprit, the severe acute respiratory syndrome coronavirus 2 has been brought under scrutiny. In addition to inhalation transmission, the possible fecal-oral viral transmission via water/wastewater has also been brought under the spotlight, necessitating a timely global review on the current knowledge about waterborne viruses in drinking water treatment system – the very barrier that intercepts waterborne pathogens to terminal water users. In this article we reviewed the occurrence, concentration methods, and control strategies, also, treatment performance on waterborne viruses during drinking water treatment were summarized. Additionally, we emphasized the potential of applying the quantitative microbial risk assessment to guide drinking water treatment to mitigate the viral exposure risks, especially when the unregulated novel viral pathogens are of concern. This review paves road for better control of viruses at drinking water treatment plants to protect public health., Graphical abstract Image 1

Chlorophenylacetonitriles (CPANs) are an emerging group of aromatic nitrogenous disinfection byproducts (DBPs). However, their dominant precursors and formation pathways remain unclear, which hinders the further development of effective control strategies. For the first time, CPAN precursors were screened by conducting formation potential (FP) tests on real water samples from six drinking water treatment plants (DWTPs). The average overall removal of CPAN precursors across all six DWTPs was only 10%. Moreover, ozonation increased CPAN precursors by 140% on average. Fluorescence spectroscopy showed a dramatic reduction in aromatic proteins, tyrosine-like proteins, and tryptophan-like proteins following ozonation. Low-apparent-molecular-weight (AMW) (

The fundamental goal of water quality engineering is to ensure water safety to humans and the environment. Traditional water quality engineering consists of monitoring, evaluation, and control of key water quality parameters. This approach provides some vital insights into water quality, however, most of these parameters do not account for pollutant mixtures - a reality that terminal water users face, nor do most of these parameters have a direct connection with the human health safety of waters. This puts the real health-specific effects of targeted water pollutant monitoring and engineering control in question. To focus our attention to one of the original goals of water quality engineering - human health and environmental protection, we advocate here the toxicity-oriented water quality monitoring and control. This article presents some of our efforts towards such goal. Specifically, complementary to traditional water quality parameters, we evaluated the water toxicity using high sensitivity toxicological endpoints, and subsequently investigated the performance of some of the water treatment strategies in modulating the water toxicity. Moreover, we implemented the toxicity concept into existing water treatment design theory to facilitate toxicity-oriented water quality control designs. Suggestions for the next steps are also discussed. We hope our work will intrigue water quality scientists and engineers to improve and embrace the mixture water pollutant and toxicological evaluation and engineering control.

An in chemico high throughput assay based on N-acetylcysteine was developed and used in conjunction with previous and new mammalian cell cytotoxicity data. Our objective was to derive an empirical equation with confidence levels for mammalian cell cytotoxicity prediction. Modeling data included 16 unique sources of waters and wastewaters of distinct water qualities to encompass a wide range of real environmental samples. This approach provides a quick screen to identify those water and wastewaters that could be prioritized for in depth analytical biological analyses and toxicity. The resulting model can serve as a preliminary convenient tool to screen for potential mammalian cell cytotoxicity in organic extracts of a wide variety of water samples.

Due to the spread of coronavirus disease 2019 (COVID-19), large amounts of antivirals were consumed and released into wastewater, posing risks to the ecosystem and human health. Ozonation is commonly utilized as pre-oxidation process to enhance the disinfection of hospital wastewater during COVID-19 spread. In this study, the transformation of ribavirin, antiviral for COVID-19, during ozone/PMS‑chlorine intensified disinfection process was investigated. •OH followed by O3 accounted for the dominant ribavirin degradation in most conditions due to higher reaction rate constant between ribavirin and •OH vs. SO4•− (1.9 × 109 vs. 7.9 × 107 M−1 s−1, respectively). During the O3/PMS process, ribavirin was dehydrogenated at the hydroxyl groups first, then lost the amide or the methanol group. Chloride at low concentrations (e.g., 0.5– 2 mg/L) slightly accelerated ribavirin degradation, while bromide, iodide, bicarbonate, and dissolved organic matter all reduced the degradation efficiency. In the presence of bromide, O3/PMS process resulted in the formation of organic brominated oxidation by-products (OBPs), the concentration of which increased with increasing bromide dosage. However, the formation of halogenated OBPs was negligible when chloride or iodide existed. Compared to the O3/H2O2 process, the concentration of brominated OBPs was significantly higher after ozonation or the O3/PMS process. This study suggests that the potential risks of the organic brominated OBPs should be taken into consideration when ozonation and ozone-based processes are used to enhance disinfection in the presence of bromide amid COVID-19 pandemic., Graphical abstract Unlabelled Image

Hydroxyl radicals (HO·) and sulfate radicals (SO4 −) can be generated when ferric-based coagulants are coupled with the potential alternative pre-oxidant peroxymonosulfate (PMS). Although HO·, SO4 − and PMS may oxidize most organic matter, they could also react with chloride stemming from chloride-containing coagulants, generating reactive chlorine species that may further react with organic matter to produce unwanted byproducts. CX3R-type [X = H or Cl, R = H, CN, C(OH)2 or CONH2] byproducts have cytotoxicity and genotoxicity. Therefore, the dissolved organic carbon (DOC) removal and CX3R-type byproduct formation during the PMS pre-oxidation followed by coagulation (PPFC) (ferric sulfate [Fe2(SO4)3], ferric chloride (FeCl3), aluminium sulfate [Al2(SO4)3] or aluminium chloride (AlCl3)) were investigated. Results showed that PPFC could remove DOC higher compared to PMS pre-oxidation or coagulation alone. The DOC removal efficiency followed the order of Fe2(SO4)3 > FeCl3 > Al2(SO4)3 > AlCl3 during the PPFC. During the PPFC, FeCl3 and AlCl3 resulted in the formation of CX3R-type byproduct that posed significant calculated toxicity induction, while Fe2(SO4)3 and Al2(SO4)3 did not. Compared to AlCl3, FeCl3 resulted in higher CX3R-type byproduct concentration and finished water toxicity, which both decreased as the pre-oxidation duration extended, and increased as the PMS concentration increased. The CX3R-type byproduct formation and finished water toxicity increased and then decreased as both sedimentation time and coagulant dosage increased. Compared to PMS and SO4 −, HO· played a more significant role in the formation of CX3R-type byproduct and induction of toxicity of finished water during the PPFC (FeCl3). Therefore, Fe2(SO4)3 was the more suitable coagulant when PMS was used as the pre-oxidant.

Water reuse is receiving unprecedented attention as many areas around the globe attempt to better-manage their fresh water resources. Wastewaters in coastal regions may contain elevated levels of bromide (Br–) and iodide (I–) from seawater intrusion or high mineral content in the source waters. Disinfection of such wastewater is essential to prevent the spread of pathogens; however, little is known about the toxicity of the treated wastewater. In this study, we evaluated the genotoxicity to Chinese hamster ovary (CHO) cells induced by municipal secondary wastewater effluent amended with elevated Br– and I– after disinfection by chlorine, chloramines, or ozone. We calibrated and applied an N-acetylcysteine (NAC) thiol reactivity assay as a surrogate for thiol reactivity with biological proteins (glutathione) of wastewater samples. Chlorination of wastewaters produced CHO cell genotoxicity comparable to chloramination, 3.9 times more genotoxic than the nondisinfected controls. Ozonated wastewater was at lea...

Drinking water utilities will increasingly rely on alternative water sources in the future, including wastewater reuse. Safety must be assured in the application of advanced oxidation processes (AOPs) and supporting treatments for wastewater effluent reuse. This study developed toxicological profiles for source and tap waters, wastewaters, and treated effluents by different processes from four military installation locations. The objective of this study was to evaluate the toxicity of extracted organics from diverse source waters and after reuse treatments. The toxicity analyses included thiol reactivity, mammalian cell cytotoxicity, and genotoxicity. Differences in toxicity between source or tap waters and effluents from wastewater treatment processes supported AOP treatment to reduce risks of potable reuse. An anoxic and aerobic activated sludge process followed by sand filtration controlled toxicity to levels similar to a municipal drinking water. An anaerobic membrane bioreactor process exceeded the toxicity levels of a typical drinking water. Two AOP processes (ultraviolet (UV) + reverse osmosis (RO) + chlorination (NaOCl) or RO + UV-H2O2 + NaOCl) significantly reduced toxicity. The integration of the wastewater systems with ultrafiltration, AOP, and RO was effective to reduce the toxicity to levels comparable to, or better than, tap water samples.

Wastewater reuse is becoming increasingly common, and there is a need for decentralized and small-scale systems to support the safe recovery of water resources. In this study, an integrated life cycle assessment (LCA) and quantitative microbial risk assessment (QMRA) were used to compare microplasma ozonation (an emerging technology) to chlorination (an established technology) for the disinfection of wastewater for landscape irrigational reuse. Three waterborne pathogens, Legionella pneumophila, Giardia, and Cryptosporidium parvum, were selected to include bacteria and protozoans covering the transmission routes of inhalation and ingestion. Inactivation data from the literature were coupled with bench-scale experiments (to establish inactivation parameters for L. pneumophila by ozone in wastewater) for the design and simulation of disinfection processes. Microplasma-based ozonation reduced more life cycle human health impacts as compared to chlorination for five of the six impact categories, because of the high susceptibility of the pathogens to ozone and the lower impacts stemming from electricity (required in ozonation) vs. chemical production (required in chlorination). These results were consistent across the electricity-fuel mixes of all fifty U.S. states. These results indicate that from the point of view of reducing human health impact, the emerging microplasma ozonation technology is superior to chlorination for wastewater reuse disinfection. To reduce the overall human health impact, future design efforts should focus on reducing process consumables (i.e., chemical and electricity consumption) through longer hydraulic residence times (HRTs), while maintaining adequate disinfectant dosing to provide reliable disinfection efficacy despite influent variability in compounds that may quench or interfere with the disinfectant.

Reusing wastewater in agriculture is becoming increasingly common, which necessitates disinfection to ensure reuse safety. However, disinfectants can react with wastewater constituents to form disinfection byproducts (DBPs), many of which are toxic and restrict the goal of safe reuse. Our objective was to benchmark the induction of mammalian cell cytotoxicity after ozonation against chlorination for three types of real wastewaters: municipal secondary effluent and two sources of minimally treated swine farm wastewaters. A new method to evaluate samples of suspected high cytotoxicity was devised. For the secondary effluent, ozonation reduced the cytotoxicity by as much as 10 times; chlorination lowered the cytotoxicity only when followed by dechlorination. The swine farm wastewaters were up to 2000 times more cytotoxic than the secondary effluent, and the highest reduction in cytotoxicity was 17 times as achieved by ozonation. These results indicate that secondary effluent is preferred over swine wastewaters for agricultural reuse regardless of the tested disinfectants. Ozonation consistently reduced the cytotoxicity of both the full strength and the organic extracts of all tested wastewaters more than chlorination. The only significant correlation was observed in the secondary wastewater between total haloacetonitriles and cytotoxicity. While the association of reduced toxicity with the modification or reduction of specific compound(s) is unclear, regulated DBPs may not be the primary forcing agents.

Toxicity arising from toxic disinfection byproducts is an unintended result of disinfection during water reclamation. To ensure safe water reclamation treatment, it is important to develop a disinfection strategy with minimal formation of overall toxicity in the reclaimed water. The cumulative disinfectant concentration over time (Ct) is a useful concept for pathogen control during reuse water disinfection. We evaluated the toxicity impact of Ct values and different methods to achieve identical Ct values by ozonation or chlorination of wastewaters from four agricultural sources on mammalian cells. N-acetylcysteine (NAC) reactivity of the wastewater organic extracts was determined to reveal their impact on the thiol-specific biological detoxification mechanism. The results demonstrated that for two sources and for both ozonation and chlorination, higher Ct values enhanced cytotoxicity. The ozonated waters were at least 10% less toxic and as much as 22.4 times less toxic than either the non-disinfected controls or the chlorinated waters. Chlorination consistently induced higher cytotoxicity than ozonation by between 2.2 and 22.4 fold, respectively, and induced similar or higher cytotoxicity than the non-disinfected controls, by at most 4.4 fold. Given the same Ct values, the combination of high disinfectant concentration and short contact time produced finished wastewaters with higher toxicity, than the combination of low disinfectant concentration and long contact time. NAC thiol reactivity was positively and significantly correlated with mammalian cell cytotoxicity, and agreed with 80% of the cytotoxicity rank order. This suggests that the induction of cytotoxicity involved reactions with agents that acted as thiol pool quenchers. The overall results indicate that the cytotoxicity of wastewaters may increase when higher Ct values are applied to inactivate recalcitrant pathogens. To counteract the potential increase in cytotoxicity at high Ct values, for both ozonation and chlorination, lower disinfectant dose and longer contact time may be adopted.

We investigated chronic mammalian cell cytotoxicity of wastewaters from four sources and their optical spectroscopic properties with or without chlorination or ozonation. Samples from effluents of activated sludge, nitrification tower, facultative waste stabilization pond, and maturation waste stabilization pond were either chlorinated or ozonated. The wastewater samples were analyzed for fluorescence excitation emission matrix, specific fluorescence index (SFI), and specific UV absorbance at 254 nm (SUVA). Before and after disinfection the wastewater samples were quantitatively analyzed for in vitro mammalian cell cytotoxicity. We found that the organic extracts from the ozonated samples induced lower cytotoxicity responses than those from the chlorinated or the nondisinfected samples. To develop correlations between SFI, SUVA, and cytotoxicity, we analyzed 21 independent samples. Significant linear correlations found among these samples suggest that under the tested conditions, cytotoxicity was preferentially influenced by the fluorescence and SUVA of their composite organic agents. These two spectroscopic parameters may be used as indicators for the potential cytotoxicity of nondisinfected, ozonated, or chlorinated municipal wastewaters.

Cryptosporidium parvum oocysts have been known to cause adverse health effects worldwide, and processes that contribute to their inactivation have gained wide attention in recent years. Solar inactivation is an important process that can improve surface water quality. Solar disinfection (SODIS) can be used to disinfect water as a point-of-use alternative, and disinfect wastewater in waste stabilization ponds. However, a clear understanding of the oocyst solar inactivation mechanisms is lacking. This study systematically investigated the oocyst solar inactivation mechanisms in the presence of a wide range of environmental factors and also provided an insight on the metabolic response of oocysts using the microarray analysis. The result revealed that oocyst inactivation by solar UVA/visible light was dominated by UVA-induced internal radical damages and was sensitive to both the temperature and the oocyst source. External radical producing sensitizers did not enhance the UVA/visible light inactivation of oocysts due to the protection by the oocyst wall. In contrast, UVB was found to directly damage the oocyst genome, ensuring an effective inactivation that correlated only with UV fluence after being corrected for light screening regardless of the oocyst source, temperature, and the presence of external sensitizers. Further microarray analysis suggested that the effective UVB inactivation could be explained by the down-regulation of most of the genes responsible for cellular metabolic activities and the lack of expression of stress protection mechanisms in oocysts after 30 minutes of UVB exposure. These results facilitate the understanding and design of water and wastewater treatment processes that involve natural sunlight exposure.