Tracing the contamination origins in water sources and identifying the impacts of natural and human processes are essential for ecological safety and public health.However,current analysis approaches are not ideal,as ...Tracing the contamination origins in water sources and identifying the impacts of natural and human processes are essential for ecological safety and public health.However,current analysis approaches are not ideal,as they tend to be laborious,time-consuming,or technically difficult.Disinfection byproducts(DBPs)are a family of well-known secondary pollutants formed by the reactions of chemical disinfectants with DBP precursors during water disinfection treatment.Since DBP precursors have various origins(e.g.,natural,domestic,industrial,and agricultural sources),and since the formation of DBPs from different precursors in the presence of specific disinfectants is distinctive,we argue that DBPs and DBP precursors can serve as alternative indicators to assess the contamination in water sources and identify pollution origins.After providing a retrospective of the origins of DBPs and DBP precursors,as well as the specific formation patterns of DBPs from different precursors,this article presents an overview of the impacts of various natural and anthropogenic factors on DBPs and DBP precursors in drinking water sources.In practice,the DBPs(i.e.,their concentration and speciation)originally present in source water and the DBP precursors determined using DBP formation potential tests—in which water samples are dosed with a stoichiometric excess of specific disinfectants in order to maximize DBP formation under certain reaction conditions—can be considered as alternative metrics.When jointly used with other water quality parameters(e.g.,dissolved organic carbon,dissolved organic nitrogen,fluorescence,and molecular weight distribution)and specific contaminants of emerging concern(e.g.,certain pharmaceuticals and personal care products),DBPs and DBP precursors in drinking water sources can provide a more comprehensive picture of water pollution for better managing water resources and ensuring human health.展开更多
The effects of ozonation on the formation potential of typical disinfection byproducts (DBPs) and the changes of genotoxicity during post chlorination of tertiary effluent from a sewage treatment plant were investig...The effects of ozonation on the formation potential of typical disinfection byproducts (DBPs) and the changes of genotoxicity during post chlorination of tertiary effluent from a sewage treatment plant were investigated. Ozonation enhanced the yields of all detected chlorine DBPs except CHCI3. At a chlorine dose of 5 mg/L, the three brominated THMs and five HAAs increased, while chloroform decreased with the increase of ozone dose from 0 to 10 mg/L (ozone dose in consumption base). At a chlorine dose of 10 mg/L, the two mixed bromochloro species THMs and two dominant HAAs (DCAA and TCAA) increased firstly and then decreased with the increase of ozone dose, with the turning point approximately occurring at an ozone dose of 5 mg/L. The genotoxicity detected using umu test, on the other hand, was removed from 7 Ixg 4-NQO/L to a negligible level by ozonation under an ozone dose of 5 mg/L. Chlorination could further remove the genotoxicity to some extent. It was found that SUVA (UV absorbance divided by DOC concentration) might be used as an indicative parameter for monitoring the removal of genotoxicity during the oxidation.展开更多
Chlorine-based sanitizers have seen wide spread use in food sanitation. The reaction of chlorine species with organic matter is a concern for two reasons. Available chlorine can be “used up” by organic compounds res...Chlorine-based sanitizers have seen wide spread use in food sanitation. The reaction of chlorine species with organic matter is a concern for two reasons. Available chlorine can be “used up” by organic compounds resulting in a lower amount of chlorine available for disinfection. Another concern is that some forms of chlorine can react with some organic compounds to form toxic halogenated disinfection byproducts(DBPs). Many studies have been conducted to evaluate the role of hypochlorous acid(HOCl) and hypochlorite ion(OCl–) in the production of DBPs with a particular interest in the production of trihalomethanes(THMs) and haloacetic acids(HAAs). Since most of the chlorine reactions are pH dependent, pH is found to have a significant effect on the formation of chlorine DBPs. In many cases, the concentration of THMs decreases and HAAs increases as pH decreases. pH also plays an important role in the determination of the type and amount of DBPs formed, with lower, more acidic, pHs resulting in the formation of less chloroform. This review summarizes the information from the literature on the role of chlorine-based sanitizers as affected by pH in the formation of different types of DBPs. Alternative novel strategies to minimize the formation of DBPs are also discussed.展开更多
Although disinfection byproducts(DBPs) in drinking water have been suggested as a cancer causing factor, the causative compounds have not yet been clarified. In this study, we used liquid chromatography quadrupole-tim...Although disinfection byproducts(DBPs) in drinking water have been suggested as a cancer causing factor, the causative compounds have not yet been clarified. In this study, we used liquid chromatography quadrupole-time-of-flight spectrometry(LC-QTOF MS) to identify the unknown disinfection byproducts(DBPs) in drinking water produced from Taihu Lake source water, which is known as a convergence point for the anthropogenic pollutants discharged from intensive industrial activities in the surrounding regions. In total, 91 formulas of DBPs were discovered through LC-QTOF MS nontarget screen, 81 of which have not yet been reported. Among the 91 molecules, 56 only contain bromine, 15 only contain chlorine and 20 DBPs have both bromine and chlorine atoms. Finally, five DBPs including 2,4,6-tribromophenol, 2,6-dibromo-4-chlorophenol, 2,6-dichloro-4-bromophenol, 4-bromo-2,6-di-tert-butylphenol and 3,6-dibromocarbazole were confirmed using standards. The former three compounds mainly formed in the predisinfection step(maximum concentration, 0.2-2.6 μg/L), while the latter two formed in the disinfection step(maximum concentration, 18.2-33.6 ng/L). In addition, 19 possible precursors of the discovered DBPs were detected, with the aromatic compounds being a major group. 2,6-di-tert-butylphenol as the precursor of 4-bromo-2,6-di-tert-butylphenol was confirmed with standard, with a concentration of 20.3 μg/L in raw water. The results of this study show that brominated DBPs which are possibly formed from industrial pollutants are relevant DBP species in drinking water produced form Taihu source water, suggesting protection of Taihu Lake source water is important to control the DBP risks.展开更多
The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typica...The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typical drinking water sources of Shanghai, were used for the investigation. Compared with the samples from Huangpu River, the raw water samples from Yangtze River had lower content of total organic carbon (TOC) and ferric ions, but higher bromide concentrations. Under controlled chlorination conditions, four trihalomethanes (THMs), nine haloacetic acids (HAAs), total organic halogen (TOX) and its halogen species fractions, including total organic chlorine (TOC1) and total organic bromide (TOBr), were determined. The results showed that co-existent ferric and bromide ions significantly promoted the formation of total THMs and HAAs for both raw water samples. Higher concentration of bromide ions significantly changed the speciation of the formed THMs and HAAs. There was an obvious shift to brominated species, which might result in a more adverse influence on the safety of drinking water. The results also indicated that high levels of bromide ions in raw water samples produced higher percentages of unknown TOBr.展开更多
Disinfection by-products (DBPs) are regulated in drinking water in a number of countries. This critical review focuses on the issues associated with DBP regulatory compliance, including methods for DBP analysis, occ...Disinfection by-products (DBPs) are regulated in drinking water in a number of countries. This critical review focuses on the issues associated with DBP regulatory compliance, including methods for DBP analysis, occurrence levels, the regulation comparison among various countries, DBP compliance strategies, and emerging DBPs. The regulation comparison between China and the United States (US) indicated that the DBP regulations in China are more stringent based on the number of regulated compounds and maximum levels. The comparison assessment using the Information Collection Rule (ICR) database indicated that the compliance rate of 500 large US water plants under the China regulations is much lower than that under the US regulations (e.g. 62.2% versus 89.6% for total trihalomethanes). Precursor removal and alternative disinfectants are common practices for DBP regulatory compliance. DBP removal after formation, including air stripping for trihalomethane removal and biodegradation for haloacetic acid removal, have gained more acceptance in DBP control. Formation of emerging DBPs, including iodinated DBPs and nitrogenous DBPs, is one of unintended consequences of precursor removal and alternative disinfection. At much lower levels than carbonaceous DBPs, however, emerging DBPs have posed higher health risks.展开更多
Eight typical drinking water supplies in China were selected in this study.Both source and tap water were used to investigate the occurrence of chlorinated disinfection byproducts(DBPs),and seasonal variation in the...Eight typical drinking water supplies in China were selected in this study.Both source and tap water were used to investigate the occurrence of chlorinated disinfection byproducts(DBPs),and seasonal variation in the concentrations of trihalomethanes(THMs) of seven water sources was compared.The results showed that the pollution level for source water in China,as shown by DBP formation potential,was low.The most encountered DBPs were chloroform,dichloroacetic acid,trichloroacetic acid,and chlorodibromoacetic acid.The concentration of every THMs and haloacetic acid(HAA) compound was under the limit of standards for drinking water quality.The highest total THMs concentrations were detected in spring.展开更多
Halobenzoquinones(HBQs)are highly toxic disinfection byproducts(DBPs)and are also precursors of other DBPs such as trihalomethanes(THMs).The formation of THMs from HBQs during chlorine-only and UV/chlorine processes w...Halobenzoquinones(HBQs)are highly toxic disinfection byproducts(DBPs)and are also precursors of other DBPs such as trihalomethanes(THMs).The formation of THMs from HBQs during chlorine-only and UV/chlorine processes with or without bromide was investigated experimentally.Density functional theory(DFT)reactivity descriptors were also applied to predict the nucleophilic/electrophilic reactive sites on HBQs and intermediates.The results were combined to explain the different behaviors of 2,6-dichloro-1,4-benzoquinone(2,6-DCBQ)and tetrachloro-1,4-benzoquinone(TCBQ)and to propose mechanism for the promoting roles of UV and hydroxylation of HBQs in THMs formation.Under UV/chlorine,UV significantly enhanced THMs formation from 2,6-DCBQ compared to chlorine-only,mainly due to the production of OH-DCBQ^(*).Excited 2,6-DCBQ^(*)by UV benefited nucleophilic hydrolysis to produce OH-DCBQ^(*),which favored electrophilic attack by chlorine,thereby inducing more THMs formation.UV/chlorine modestly promoted THMs formation from TCBQ compared to chlorine-only.Hydroxylation of TCBQ and UV irradiation were both important in promoting THMs formation due to the high electrophilic property of OH-TCBQ and TCBQ^(*).Meanwhile,hydroxylation of HBQs and CHCl3 formation were enhanced at higher pH.This work suggested that enhanced formation of THMs from HBQs should be considered in the application of combined UV and chlorine processes.展开更多
Algal blooms and wastewater effluents can introduce algal organic matter(AOM) and effluent organic matter(Ef OM) into surface waters, respectively. In this study, the impact of bromide and iodide on the formation of h...Algal blooms and wastewater effluents can introduce algal organic matter(AOM) and effluent organic matter(Ef OM) into surface waters, respectively. In this study, the impact of bromide and iodide on the formation of halogenated disinfection byproducts(DBPs) during chlorination and chloramination from various types of dissolved organic matter(DOM, e.g., natural organic matter(NOM), AOM, and Ef OM) were investigated based on the data collected from literature. In general, higher formation of trihalomethanes(THMs) and haloacetic acids(HAAs) was observed in NOM than AOM and Ef OM, indicating high reactivities of phenolic moieties with both chlorine and monochloramine. The formation of haloacetaldehydes(HALs), haloacetonitriles(HANs) and haloacetamides(HAMs) was much lower than THMs and HAAs. Increasing initial bromide concentrations increased the formation of THMs, HAAs, HANs, and HAMs, but not HALs. Bromine substitution factor(BSF) values of DBPs formed in chlorination decreased as specific ultraviolet absorbance(SUVA) increased. AOM favored the formation of iodinated THMs(I-THMs) during chloramination using preformed chloramines and chlorination-chloramination processes. Increasing prechlorination time can reduce the I-THM concentrations because of the conversion of iodide to iodate, but this increased the formation of chlorinated and brominated DBPs. In an analogous way, iodine substitution factor(ISF) values of I-THMs formed in chloramination decreased as SUVA values of DOM increased. Compared to chlorination, the formation of noniodinated DBPs is low in chloramination.展开更多
Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving...Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving water treatment practices have led to a continually growing list of DBPs.Advancement of analytical technologies have enabled the identification of new classes of DBPs and the quantification of these chemically diverse sets of DBPs.Here we summarize advances in new workflows for DBP analysis,including sample preparation,chromatographic separation with mass spectrometry(MS)detection,and data processing.To aid in the selection of techniques for future studies,we discuss necessary considerations for each step in the strategy.This review focuses on how each step of a workflow can be optimized to capture diverse classes of DBPs within a single method.Additionally,we highlight new MS-based approaches that can be powerful for identifying novel DBPs of toxicological relevance.We discuss current challenges and provide perspectives on future research directions with respect to studying new DBPs of toxicological relevance.As analytical technologies continue to advance,new strategies will be increasingly used to analyze complex DBPs produced in different treatment processes with the aim to identify potential drivers of toxicity.展开更多
Chlorination is essential to the safety of reclaimed water; however, this process leads to concern regarding the formation of disinfection byproducts(DBPs) and toxicity. This study reviewed the formation and control...Chlorination is essential to the safety of reclaimed water; however, this process leads to concern regarding the formation of disinfection byproducts(DBPs) and toxicity. This study reviewed the formation and control strategies for DBPs and toxicity in reclaimed water during chlorination.Both regulated and emerging DBPs have been frequently detected in reclaimed water during chlorination at a higher level than those in drinking water, indicating they pose a greater risk to humans. Luminescent bacteria and Daphnia magna acute toxicity, anti-estrogenic activity and cytotoxicity generally increased after chlorination because of the formation of DBPs. Genotoxicity by umu-test and estrogenic activity were decreased after chlorination because of destruction of toxic chemicals. During chlorination, water quality significantly impacted changes in toxicity.Ammonium tended to attenuate toxicity changes by reacting with chlorine to form chloramine,while bromide tended to aggravate toxicity changes by forming hypobromous acid. During pretreatment by ozonation and coagulation, disinfection byproduct formation potential(DBPFP)and toxicity formation potential(TFP) occasionally increase, which is accompanied by DOC removal; thus, the decrease of DOC was limited to indicate the decrease of DBPFP and TFP. It is more important to eliminate the key fraction of precursors such as hydrophobic acid and hydrophilic neutrals. During chlorination, toxicities can increase with the increasing chlorine dose and contact time. To control the excessive toxicity formation, a relatively low chlorine dose and short contact time were required. Quenching chlorine residual with reductive reagents also effectively abated the formation of toxic compounds.展开更多
The chemistry associated with the disinfection of aquarium seawater is more complicated than that of freshwater, therefore limited information is available on the formation and speciation of disinfection byproducts(D...The chemistry associated with the disinfection of aquarium seawater is more complicated than that of freshwater, therefore limited information is available on the formation and speciation of disinfection byproducts(DBPs) in marine aquaria. In this study, the effects of organic precursors, bromide(Br-) and pre-ozonation on the formation and speciation of several typical classes of DBPs, including trihalomethanes(THM4), haloacetic acids(HAAs),iodinated trihalomethanes(I-THMs), and haloacetamides(HAc Ams), were investigated during the chlorination/chloramination of aquarium seawater. Results indicate that with an increase in dissolved organic carbon concentration from 4.5 to 9.4 mg/L, the concentrations of THM4 and HAAs increased by 3.2-7.8 times under chlorination and by 1.1-2.3 times under chloramination. An increase in Br-concentration from 3 to 68 mg/L generally enhanced the formation of THM4, I-THMs and HAc Ams and increased the bromine substitution factors of all studied DBPs as well, whereas it impacted insignificantly on the yield of HAAs. Pre-ozonation with 1 mg/L O3 dose substantially reduced the formation of all studied DBPs in the subsequent chlorination and I-THMs in the subsequent chloramination. Because chloramination produces much lower amounts of DBPs than chlorination, it tends to be more suitable for disinfection of aquarium seawater.展开更多
The reclamation and disinfection of waters impacted by human activities(e.g., wastewater effluent discharges) are of growing interest for various applications but has been associated with the formation of toxic nitr...The reclamation and disinfection of waters impacted by human activities(e.g., wastewater effluent discharges) are of growing interest for various applications but has been associated with the formation of toxic nitrogenous disinfection byproducts(N-DBPs). Monochloramine used as an alternative disinfectant to chlorine can be an additional source of nitrogen in the formation of N-DBPs. Individual toxicity assays have been performed on many DBPs, but few studies have been conducted with complex mixtures such as wastewater effluents. In this work, we compared the cytotoxicity and genotoxicity of wastewater effluent organic matter(Ef OM) before and after chloramination. The toxicity of chloraminated Ef OM was significantly higher than the toxicity of raw Ef OM, and the more hydrophobic fraction(HPO)isolated on XAD-8 resin was more toxic than the fraction isolated on XAD-4 resin.More DBPs were also isolated on the XAD-8 resin. N-DBPs(i.e., haloacetonitriles or haloacetamides) were responsible for the majority of the cytotoxicity estimated from DBP concentrations measured in the XAD-8 and XAD-4 fractions(99.4% and 78.5%, respectively).Measured DBPs accounted for minor proportions of total brominated and chlorinated products, which means that many unknown halogenated compounds were formed and can be responsible for a significant part of the toxicity. Other non-halogenated byproducts(e.g.,nitrosamines) may contribute to the toxicity of chloraminated effluents as well.展开更多
Human neural stem cells(h NSCs) are a useful tool to assess the developmental effects of various environmental contaminants; however, the application of h NSCs to evaluate water disinfection byproducts(DBPs) is sc...Human neural stem cells(h NSCs) are a useful tool to assess the developmental effects of various environmental contaminants; however, the application of h NSCs to evaluate water disinfection byproducts(DBPs) is scarce. Comprehensive toxicological results are essential to the prioritization of DBPs for further testing and regulation. Therefore, this study examines the effects of DBPs on the proliferation and differentiation of h NSCs. Prior to DBP treatment, characteristic protein markers of h NSCs from passages 3 to 6 were carefully examined and it was determined that h NSCs passaged 3 or 4 times maintained stem cell characteristics and can be used for DBP analysis. Two regulated DBPs, monobromoacetic acid(BAA) and monochloroacetic acid(CAA), and two emerging DBPs, 2,6-dibromo-1,4-benzoquinone(2,6-DBBQ) and 2,6-dichloro-1,4-benzoquinone(2,6-DCBQ), were chosen for h NSC treatment. Both 2,6-DBBQ and 2,6-DCBQ induced cell cycle arrest at S-phase at concentrations up to 1 μmol/L. Comparatively, BAA and CAA at 0.5 μmol/L affected neural differentiation. These results suggest DBP-dependent effects on h NSC proliferation and differentiation. The DBP-induced cell cycle arrest and inhibition of normal h NSC differentiation demonstrate the need to assess the developmental neurotoxicity of DBPs.展开更多
When bromide/iodide is present in source water, hypobromous acid/hypoiodous acid will be formed with addition of chlorine, chloramine, or other disinfectants. Hypobromous acid/hypoiodous acid undergoes reactions with ...When bromide/iodide is present in source water, hypobromous acid/hypoiodous acid will be formed with addition of chlorine, chloramine, or other disinfectants. Hypobromous acid/hypoiodous acid undergoes reactions with natural organic matter in source water to form numerous brominated/iodinated disinfection byproducts (DBPs). In this study, tap water samples were collected from eight cities in China. With the aid of electrospray ionization-triple quadrupole mass spectrometry by setting precursor ion scans of m/z 35, m/z 81, and m/z 126.9, whole pictures of polar chlorinated, brominated, and iodinated DBPs in the tap water samples were revealed for the first time. Numerous polar halogenated DBPs were detected, including haloacetic acids, newly identified halogenated phenols, and many new/unknown halogenated compounds. Total organic chlorine, total organic bromine, and total organic iodine were also measured to indicate the total levels of all chlorinated, brominated, and iodinated DBPs in the tap water samples. The total organic chlorine concentrations ranged from 26.8 to 194.0 μg· L 1 as Cl, with an average of 109.2 μg·L-1 as Cl; the total organic bromine concentrations ranged from below detection limit to 113.3 μg·L-1 as Br, with an average of 34.7 μg·L-1 as Br; the total organic iodine concentrations ranged from below detection limit to 16.4 μg· L-1 as I, with an average of 9.1 μg· L-1 as I; the total organic halogen concentrations ranged from 31.3 to 220.4 μg·L-1 as Cl, with an average of 127.2 μg· L- 1 as Cl.展开更多
In the race to deliver clean water to communities through potable water reuse, disinfection and water quality assessment are and will continue to be fundamental factors. There are over 700 disinfection byproducts(DBPs...In the race to deliver clean water to communities through potable water reuse, disinfection and water quality assessment are and will continue to be fundamental factors. There are over 700 disinfection byproducts(DBPs) in water;evaluating each compound is practically impossible and very time consuming. A bioanalytical approach could be an answer to this challenge. In this work, the response of four major classes of DBPs toward mitochondrial membrane potential( Δψm) and cytoplasmic adenosine triphosphate(C-ATP) was investigated with human carcinoma(Hep G2) cells. Within 90 min of cell exposure, only the haloacetic acid(HAA) mixture caused a cytotoxic response as measured by C-ATP. All four groups(haloacetonitriles(HANs), trihalomethanes(THMs), nitrosamines(NOAs), and HAAs) responded well to Δψm, R 2 > 0.70. Based on the half-maximum concentration that evoked a 50% response in Δψm, the response gradient was HANs >> HAAs ~ THM > NOAs. The inhibition of the Δψm by HANs is driven by dibromoacetonitrile(DBAN), while dichloroacetonitrile(DCAN) did not cause a significant change in the Δψm at less than 2000 μM. A mixture of HANs exhibited an antagonistic behavior on the Δψm compared to individual compounds. If water samples are concentrated to increase HAN concentrations, especially DBAN, then Δψm could be used as a biomonitoring tool for DBP toxicity.展开更多
Disinfection byproducts (DBPs) are emerging pollutants in drinking water with high health risks. Precursor reduction before disinfection is an effective strategy to control the formation of DBPs. In this study, three ...Disinfection byproducts (DBPs) are emerging pollutants in drinking water with high health risks. Precursor reduction before disinfection is an effective strategy to control the formation of DBPs. In this study, three types of anion exchange resins (AERs) and two types of nanofiltration (NF) membranes were tested for their control effects on DBP precursors, DBPs, and total organic halogen (TOX). The results showed that, for AER adsorption, the removal efficiencies of DBP precursors, DBPs, and TOX increased with the increase of resin dose, and the strong basic macroporous anion exchange resin (M500MB) had the highest removal efficiencies. For NF, the highest removal efficiencies were achieved at an operating pressure of 4 bar, and the membrane (NF90) with a smaller molecular weight cut-off, had a better control efficiency. However, AER adsorption was inefficient in removing dissolved organic carbon (DOC);NF was inefficient in removing Br− resulting in insufficient control of Br-DBPs. Accordingly, a sequential approach of AER (M500MB) adsorption followed by NF (NF90) was developed to enhance the control efficiency of DBPs. Compared with single AER adsorption and single NF, the sequential approach further increased the removal efficiencies of DOC by 19.4%–101.9%, coupled with the high Br− removal efficiency of 92%, and thus improved the reduction of cyclic DBPs and TOX by 3.5%–4.9%, and 2.4%–8.4%, respectively;the sequential approach also reduced the cytotoxicity of the water sample by 66.4%.展开更多
A broad range of organic compounds are known to exist in drinking water sources and serve as precursors of disinfection byproducts(DBPs).Epidemiological findings of an association of increased risk of bladder cancer...A broad range of organic compounds are known to exist in drinking water sources and serve as precursors of disinfection byproducts(DBPs).Epidemiological findings of an association of increased risk of bladder cancer with the consumption of chlorinated water has resulted in health concerns about DBPs.Peptides are thought to be an important category of DBP precursors in water.However,little is known about the actual presence of peptides and their DBPs in drinking water because of their high sample complexity and low concentrations.To address this challenge and identify peptides and non-chlorinated/chlorinated peptide DBPs from large sets of organic compounds in water,we developed a novel high throughput analysis strategy,which integrated multiple solid phase extraction(SPE),high performance liquid chromatography(HPLC)separation,and non-target identification using precursor ion exclusion(PIE)high resolution mass spectrometry(MS).After MS analysis,structures of candidate compounds,particularly peptides,were obtained by searching against the Human Metabolome Database(HMDB).Using this strategy,we successfully detected 625 peptides(out of 17,205 putative compounds)and 617 peptides(out of 13,297)respectively in source and finished water samples.The source and finished water samples had 501 peptides and amino acids in common.The remaining 116 peptides and amino acids were unique to the finished water.From a subset of 30 putative compounds for which standards were available,25 were confirmed using HPLC-MS analysis.By analyzing the peptides identified in source and finished water,we successfully confirmed three disinfection reaction pathways that convert peptides into toxic DBPs.展开更多
Chlorine, chlorine dioxide, and ozone are widely used as disinfectants in drinking water treatments. However, the combined use of different disinfectants can result in the formation of various organic and inorganic di...Chlorine, chlorine dioxide, and ozone are widely used as disinfectants in drinking water treatments. However, the combined use of different disinfectants can result in the formation of various organic and inorganic disinfection byproducts(DBPs). The toxic interactions, including synergism, addition, and antagonism, among the complex DBPs are still unclear. In this study, we established and verified a real-time cell analysis(RTCA) method for cytotoxicity measurement on Chinese hamster ovary(CHO) cell. Using this convenient and accurate method, we assessed the cytotoxicity of a series of binary combinations consisting of one of the 3 inorganic DBPs(chlorite, chlorate, and bromate) and one of the 32 regulated and emerging organic DBPs. The combination index(CI) of each combination was calculated and evaluated by isobolographic analysis to reflect the toxic interactions. The results confirmed the synergistic effect on cytotoxicity in the binary combinations consisting of chlorite and one of the 5 organic DBPs(2 iodinated DBPs(I-DBPs) and 3 brominated DBPs(Br-DBPs)), chlorate and one of the 4 organic DBPs(3 aromatic DBPs and dibromoacetonitrile), and bromate and one of the 3 organic DBPs(2 I-DBPs and dibromoacetic acid). The possible synergism mechanism of organic DBPs on the inorganic ones may be attributed to the influence of organic DBPs on cell membrane and cell antioxidant system. This study revealed the toxic interactions among organic and inorganic DBPs, and emphasized the latent adverse outcomes in the combined use of different disinfectants.展开更多
Halogenated disinfection byproducts(DBPs) are an unintended consequence of drinking water disinfection, and can have significant toxicity. XAD resins are commonly used to extract and enrich trace levels of DBPs for co...Halogenated disinfection byproducts(DBPs) are an unintended consequence of drinking water disinfection, and can have significant toxicity. XAD resins are commonly used to extract and enrich trace levels of DBPs for comprehensive, nontarget identification of DBPs and also for in vitro toxicity studies. However, XAD resin recoveries for complete classes of halogenated DBPs have not been evaluated, particularly for low, environmentally relevant levels(ng/L to low μg/L). Thus, it is not known whether levels of DBPs or the toxicity of drinking water might be underestimated. In this study, DAX-8/XAD-2 layered resins were evaluated, considering both adsorption and elution from the resins, for extracting 66 DBPs from water. Results demonstrate that among the 7 classes of DBPs investigated, trihalomethanes(THMs), including iodo-THMs, were the most efficiently adsorbed, with recovery of most THMs ranging from 50%-96%, followed by halonitromethanes(40%-90%). The adsorption ability of XAD resins for haloacetonitriles, haloacetamides, and haloacetaldehydes was highly dependent on the individual species. The adsorption capacity of XAD resins for haloacetic acids was lower(5%-48%), even after adjusting to p H 1 before extraction. Recovery efficiency for most DBPs was comparable with their adsorption, as most were eluted effectively from XAD resins by ethyl acetate. DBP polarity and molecular weight were the two most important factors that determine their recovery. Recovery of trichloromethane, iodoacetic acid, chloro-and iodo-acetonitrile, and chloroacetamide were among the lowest, which could lead to underestimation of toxicity, particularly for iodoacetic acid and iodo-acetonitrile, which are highly toxic.展开更多
基金supported by the National Natural Science Foundation of China(52325001,52170009,and 52091542)the National Key Research and Development Program of China(2021YFC3200700)+3 种基金the Program of Shanghai Academic Research Leader,China(21XD1424000)the International Cooperation Project of Shanghai Science and Technology Commission(20230714100)the Key-Area Research and Development Program of Guangdong Province(2020B1111350001)Tongji University Youth 100 Program.
文摘Tracing the contamination origins in water sources and identifying the impacts of natural and human processes are essential for ecological safety and public health.However,current analysis approaches are not ideal,as they tend to be laborious,time-consuming,or technically difficult.Disinfection byproducts(DBPs)are a family of well-known secondary pollutants formed by the reactions of chemical disinfectants with DBP precursors during water disinfection treatment.Since DBP precursors have various origins(e.g.,natural,domestic,industrial,and agricultural sources),and since the formation of DBPs from different precursors in the presence of specific disinfectants is distinctive,we argue that DBPs and DBP precursors can serve as alternative indicators to assess the contamination in water sources and identify pollution origins.After providing a retrospective of the origins of DBPs and DBP precursors,as well as the specific formation patterns of DBPs from different precursors,this article presents an overview of the impacts of various natural and anthropogenic factors on DBPs and DBP precursors in drinking water sources.In practice,the DBPs(i.e.,their concentration and speciation)originally present in source water and the DBP precursors determined using DBP formation potential tests—in which water samples are dosed with a stoichiometric excess of specific disinfectants in order to maximize DBP formation under certain reaction conditions—can be considered as alternative metrics.When jointly used with other water quality parameters(e.g.,dissolved organic carbon,dissolved organic nitrogen,fluorescence,and molecular weight distribution)and specific contaminants of emerging concern(e.g.,certain pharmaceuticals and personal care products),DBPs and DBP precursors in drinking water sources can provide a more comprehensive picture of water pollution for better managing water resources and ensuring human health.
基金supported by the National Natu-ral Sciences Foundation of China (No. 50525824)the Tianjin Special Innovation Fund (No. 06FZZDSH00900,TJZX1-YW03)the National Water Project (No.2008ZX07314-003)
文摘The effects of ozonation on the formation potential of typical disinfection byproducts (DBPs) and the changes of genotoxicity during post chlorination of tertiary effluent from a sewage treatment plant were investigated. Ozonation enhanced the yields of all detected chlorine DBPs except CHCI3. At a chlorine dose of 5 mg/L, the three brominated THMs and five HAAs increased, while chloroform decreased with the increase of ozone dose from 0 to 10 mg/L (ozone dose in consumption base). At a chlorine dose of 10 mg/L, the two mixed bromochloro species THMs and two dominant HAAs (DCAA and TCAA) increased firstly and then decreased with the increase of ozone dose, with the turning point approximately occurring at an ozone dose of 5 mg/L. The genotoxicity detected using umu test, on the other hand, was removed from 7 Ixg 4-NQO/L to a negligible level by ozonation under an ozone dose of 5 mg/L. Chlorination could further remove the genotoxicity to some extent. It was found that SUVA (UV absorbance divided by DOC concentration) might be used as an indicative parameter for monitoring the removal of genotoxicity during the oxidation.
文摘Chlorine-based sanitizers have seen wide spread use in food sanitation. The reaction of chlorine species with organic matter is a concern for two reasons. Available chlorine can be “used up” by organic compounds resulting in a lower amount of chlorine available for disinfection. Another concern is that some forms of chlorine can react with some organic compounds to form toxic halogenated disinfection byproducts(DBPs). Many studies have been conducted to evaluate the role of hypochlorous acid(HOCl) and hypochlorite ion(OCl–) in the production of DBPs with a particular interest in the production of trihalomethanes(THMs) and haloacetic acids(HAAs). Since most of the chlorine reactions are pH dependent, pH is found to have a significant effect on the formation of chlorine DBPs. In many cases, the concentration of THMs decreases and HAAs increases as pH decreases. pH also plays an important role in the determination of the type and amount of DBPs formed, with lower, more acidic, pHs resulting in the formation of less chloroform. This review summarizes the information from the literature on the role of chlorine-based sanitizers as affected by pH in the formation of different types of DBPs. Alternative novel strategies to minimize the formation of DBPs are also discussed.
基金This work was supported by Major Science and Technology Program for Water Pollution Control and Treatment(No.2017ZX07502003)the National Key R&D Program of China(No.2018YFE0204101).
文摘Although disinfection byproducts(DBPs) in drinking water have been suggested as a cancer causing factor, the causative compounds have not yet been clarified. In this study, we used liquid chromatography quadrupole-time-of-flight spectrometry(LC-QTOF MS) to identify the unknown disinfection byproducts(DBPs) in drinking water produced from Taihu Lake source water, which is known as a convergence point for the anthropogenic pollutants discharged from intensive industrial activities in the surrounding regions. In total, 91 formulas of DBPs were discovered through LC-QTOF MS nontarget screen, 81 of which have not yet been reported. Among the 91 molecules, 56 only contain bromine, 15 only contain chlorine and 20 DBPs have both bromine and chlorine atoms. Finally, five DBPs including 2,4,6-tribromophenol, 2,6-dibromo-4-chlorophenol, 2,6-dichloro-4-bromophenol, 4-bromo-2,6-di-tert-butylphenol and 3,6-dibromocarbazole were confirmed using standards. The former three compounds mainly formed in the predisinfection step(maximum concentration, 0.2-2.6 μg/L), while the latter two formed in the disinfection step(maximum concentration, 18.2-33.6 ng/L). In addition, 19 possible precursors of the discovered DBPs were detected, with the aromatic compounds being a major group. 2,6-di-tert-butylphenol as the precursor of 4-bromo-2,6-di-tert-butylphenol was confirmed with standard, with a concentration of 20.3 μg/L in raw water. The results of this study show that brominated DBPs which are possibly formed from industrial pollutants are relevant DBP species in drinking water produced form Taihu source water, suggesting protection of Taihu Lake source water is important to control the DBP risks.
基金supported by the National Mega-Project of Science and Technology of China (No.2008ZX07421-002)the National Eleventh Five-Year Pillar Program of Sciencethe Technology of China (No.2006BAJ04A07)
文摘The effects of ferric ion, pH, and bromide on the formation and distribution of disinfection byproducts (DBPs) during chlorination were studied. Two raw water samples from Huangpu River and Yangtze River, two typical drinking water sources of Shanghai, were used for the investigation. Compared with the samples from Huangpu River, the raw water samples from Yangtze River had lower content of total organic carbon (TOC) and ferric ions, but higher bromide concentrations. Under controlled chlorination conditions, four trihalomethanes (THMs), nine haloacetic acids (HAAs), total organic halogen (TOX) and its halogen species fractions, including total organic chlorine (TOC1) and total organic bromide (TOBr), were determined. The results showed that co-existent ferric and bromide ions significantly promoted the formation of total THMs and HAAs for both raw water samples. Higher concentration of bromide ions significantly changed the speciation of the formed THMs and HAAs. There was an obvious shift to brominated species, which might result in a more adverse influence on the safety of drinking water. The results also indicated that high levels of bromide ions in raw water samples produced higher percentages of unknown TOBr.
文摘Disinfection by-products (DBPs) are regulated in drinking water in a number of countries. This critical review focuses on the issues associated with DBP regulatory compliance, including methods for DBP analysis, occurrence levels, the regulation comparison among various countries, DBP compliance strategies, and emerging DBPs. The regulation comparison between China and the United States (US) indicated that the DBP regulations in China are more stringent based on the number of regulated compounds and maximum levels. The comparison assessment using the Information Collection Rule (ICR) database indicated that the compliance rate of 500 large US water plants under the China regulations is much lower than that under the US regulations (e.g. 62.2% versus 89.6% for total trihalomethanes). Precursor removal and alternative disinfectants are common practices for DBP regulatory compliance. DBP removal after formation, including air stripping for trihalomethane removal and biodegradation for haloacetic acid removal, have gained more acceptance in DBP control. Formation of emerging DBPs, including iodinated DBPs and nitrogenous DBPs, is one of unintended consequences of precursor removal and alternative disinfection. At much lower levels than carbonaceous DBPs, however, emerging DBPs have posed higher health risks.
基金supported by the National Natural Science Foundation of China(No.51025830,50921064)the S&T Research Project of Guangdong Province(No. 2009A080303007)the Hi-Tech Research and Development Program(863) of China(No.2006AA06Z312)
文摘Eight typical drinking water supplies in China were selected in this study.Both source and tap water were used to investigate the occurrence of chlorinated disinfection byproducts(DBPs),and seasonal variation in the concentrations of trihalomethanes(THMs) of seven water sources was compared.The results showed that the pollution level for source water in China,as shown by DBP formation potential,was low.The most encountered DBPs were chloroform,dichloroacetic acid,trichloroacetic acid,and chlorodibromoacetic acid.The concentration of every THMs and haloacetic acid(HAA) compound was under the limit of standards for drinking water quality.The highest total THMs concentrations were detected in spring.
基金supported partly by National Natural Science Foundation of China(Grant No.51978643)Youth Innovation Promotion Association,CAS(No.2014037)。
文摘Halobenzoquinones(HBQs)are highly toxic disinfection byproducts(DBPs)and are also precursors of other DBPs such as trihalomethanes(THMs).The formation of THMs from HBQs during chlorine-only and UV/chlorine processes with or without bromide was investigated experimentally.Density functional theory(DFT)reactivity descriptors were also applied to predict the nucleophilic/electrophilic reactive sites on HBQs and intermediates.The results were combined to explain the different behaviors of 2,6-dichloro-1,4-benzoquinone(2,6-DCBQ)and tetrachloro-1,4-benzoquinone(TCBQ)and to propose mechanism for the promoting roles of UV and hydroxylation of HBQs in THMs formation.Under UV/chlorine,UV significantly enhanced THMs formation from 2,6-DCBQ compared to chlorine-only,mainly due to the production of OH-DCBQ^(*).Excited 2,6-DCBQ^(*)by UV benefited nucleophilic hydrolysis to produce OH-DCBQ^(*),which favored electrophilic attack by chlorine,thereby inducing more THMs formation.UV/chlorine modestly promoted THMs formation from TCBQ compared to chlorine-only.Hydroxylation of TCBQ and UV irradiation were both important in promoting THMs formation due to the high electrophilic property of OH-TCBQ and TCBQ^(*).Meanwhile,hydroxylation of HBQs and CHCl3 formation were enhanced at higher pH.This work suggested that enhanced formation of THMs from HBQs should be considered in the application of combined UV and chlorine processes.
基金partially supported by the Key Laboratory of Drinking Water Science and Technology of Chinese Academy of Sciences (No. 20Z01KLDWST)。
文摘Algal blooms and wastewater effluents can introduce algal organic matter(AOM) and effluent organic matter(Ef OM) into surface waters, respectively. In this study, the impact of bromide and iodide on the formation of halogenated disinfection byproducts(DBPs) during chlorination and chloramination from various types of dissolved organic matter(DOM, e.g., natural organic matter(NOM), AOM, and Ef OM) were investigated based on the data collected from literature. In general, higher formation of trihalomethanes(THMs) and haloacetic acids(HAAs) was observed in NOM than AOM and Ef OM, indicating high reactivities of phenolic moieties with both chlorine and monochloramine. The formation of haloacetaldehydes(HALs), haloacetonitriles(HANs) and haloacetamides(HAMs) was much lower than THMs and HAAs. Increasing initial bromide concentrations increased the formation of THMs, HAAs, HANs, and HAMs, but not HALs. Bromine substitution factor(BSF) values of DBPs formed in chlorination decreased as specific ultraviolet absorbance(SUVA) increased. AOM favored the formation of iodinated THMs(I-THMs) during chloramination using preformed chloramines and chlorination-chloramination processes. Increasing prechlorination time can reduce the I-THM concentrations because of the conversion of iodide to iodate, but this increased the formation of chlorinated and brominated DBPs. In an analogous way, iodine substitution factor(ISF) values of I-THMs formed in chloramination decreased as SUVA values of DOM increased. Compared to chlorination, the formation of noniodinated DBPs is low in chloramination.
文摘Disinfection byproducts(DBPs)represent a ubiquitous source of chemical exposure in disinfected water.While over 700 DBPs have been identified,the drivers of toxicity remain poorly understood.Additionally,ever evolving water treatment practices have led to a continually growing list of DBPs.Advancement of analytical technologies have enabled the identification of new classes of DBPs and the quantification of these chemically diverse sets of DBPs.Here we summarize advances in new workflows for DBP analysis,including sample preparation,chromatographic separation with mass spectrometry(MS)detection,and data processing.To aid in the selection of techniques for future studies,we discuss necessary considerations for each step in the strategy.This review focuses on how each step of a workflow can be optimized to capture diverse classes of DBPs within a single method.Additionally,we highlight new MS-based approaches that can be powerful for identifying novel DBPs of toxicological relevance.We discuss current challenges and provide perspectives on future research directions with respect to studying new DBPs of toxicological relevance.As analytical technologies continue to advance,new strategies will be increasingly used to analyze complex DBPs produced in different treatment processes with the aim to identify potential drivers of toxicity.
基金funded by the National Natural Science Foundation of China (Nos.51578308, 51678332)the International S&T Cooperation Program of China (ISTCP) (No.S2016G6030)+2 种基金the National Water Pollution Control and Treatment Science and Technology Major Project (No.20122X07302002)the Shenzhen Science, Technology and Innovation Commission (No.JCYJ20160125095838752)the Collaborative Innovation Center for Regional Environmental Quality
文摘Chlorination is essential to the safety of reclaimed water; however, this process leads to concern regarding the formation of disinfection byproducts(DBPs) and toxicity. This study reviewed the formation and control strategies for DBPs and toxicity in reclaimed water during chlorination.Both regulated and emerging DBPs have been frequently detected in reclaimed water during chlorination at a higher level than those in drinking water, indicating they pose a greater risk to humans. Luminescent bacteria and Daphnia magna acute toxicity, anti-estrogenic activity and cytotoxicity generally increased after chlorination because of the formation of DBPs. Genotoxicity by umu-test and estrogenic activity were decreased after chlorination because of destruction of toxic chemicals. During chlorination, water quality significantly impacted changes in toxicity.Ammonium tended to attenuate toxicity changes by reacting with chlorine to form chloramine,while bromide tended to aggravate toxicity changes by forming hypobromous acid. During pretreatment by ozonation and coagulation, disinfection byproduct formation potential(DBPFP)and toxicity formation potential(TFP) occasionally increase, which is accompanied by DOC removal; thus, the decrease of DOC was limited to indicate the decrease of DBPFP and TFP. It is more important to eliminate the key fraction of precursors such as hydrophobic acid and hydrophilic neutrals. During chlorination, toxicities can increase with the increasing chlorine dose and contact time. To control the excessive toxicity formation, a relatively low chlorine dose and short contact time were required. Quenching chlorine residual with reductive reagents also effectively abated the formation of toxic compounds.
基金financially supported by the People Programme (Marie Curie Actions) of the European Union's Seventh Programme FP7/2007-2013 under a REA grant (No. 318926)the National Natural Science Foundation of China (No. 51221892)
文摘The chemistry associated with the disinfection of aquarium seawater is more complicated than that of freshwater, therefore limited information is available on the formation and speciation of disinfection byproducts(DBPs) in marine aquaria. In this study, the effects of organic precursors, bromide(Br-) and pre-ozonation on the formation and speciation of several typical classes of DBPs, including trihalomethanes(THM4), haloacetic acids(HAAs),iodinated trihalomethanes(I-THMs), and haloacetamides(HAc Ams), were investigated during the chlorination/chloramination of aquarium seawater. Results indicate that with an increase in dissolved organic carbon concentration from 4.5 to 9.4 mg/L, the concentrations of THM4 and HAAs increased by 3.2-7.8 times under chlorination and by 1.1-2.3 times under chloramination. An increase in Br-concentration from 3 to 68 mg/L generally enhanced the formation of THM4, I-THMs and HAc Ams and increased the bromine substitution factors of all studied DBPs as well, whereas it impacted insignificantly on the yield of HAAs. Pre-ozonation with 1 mg/L O3 dose substantially reduced the formation of all studied DBPs in the subsequent chlorination and I-THMs in the subsequent chloramination. Because chloramination produces much lower amounts of DBPs than chlorination, it tends to be more suitable for disinfection of aquarium seawater.
基金supported by the King Abdullah University of Science and Technology (KAUST) Office of Competitive Research Funds, entitled "Nitrogenous Disinfection By-Products in Reclaimed Wastewater Effluents: Chemistry, Toxicity and Control Strategies"
文摘The reclamation and disinfection of waters impacted by human activities(e.g., wastewater effluent discharges) are of growing interest for various applications but has been associated with the formation of toxic nitrogenous disinfection byproducts(N-DBPs). Monochloramine used as an alternative disinfectant to chlorine can be an additional source of nitrogen in the formation of N-DBPs. Individual toxicity assays have been performed on many DBPs, but few studies have been conducted with complex mixtures such as wastewater effluents. In this work, we compared the cytotoxicity and genotoxicity of wastewater effluent organic matter(Ef OM) before and after chloramination. The toxicity of chloraminated Ef OM was significantly higher than the toxicity of raw Ef OM, and the more hydrophobic fraction(HPO)isolated on XAD-8 resin was more toxic than the fraction isolated on XAD-4 resin.More DBPs were also isolated on the XAD-8 resin. N-DBPs(i.e., haloacetonitriles or haloacetamides) were responsible for the majority of the cytotoxicity estimated from DBP concentrations measured in the XAD-8 and XAD-4 fractions(99.4% and 78.5%, respectively).Measured DBPs accounted for minor proportions of total brominated and chlorinated products, which means that many unknown halogenated compounds were formed and can be responsible for a significant part of the toxicity. Other non-halogenated byproducts(e.g.,nitrosamines) may contribute to the toxicity of chloraminated effluents as well.
基金supported by funding from the Natural Sciences and Engineering Research Council (NSERC) of Canada, Alberta Innovates-Energy and Environmental Solutions, and Alberta Health
文摘Human neural stem cells(h NSCs) are a useful tool to assess the developmental effects of various environmental contaminants; however, the application of h NSCs to evaluate water disinfection byproducts(DBPs) is scarce. Comprehensive toxicological results are essential to the prioritization of DBPs for further testing and regulation. Therefore, this study examines the effects of DBPs on the proliferation and differentiation of h NSCs. Prior to DBP treatment, characteristic protein markers of h NSCs from passages 3 to 6 were carefully examined and it was determined that h NSCs passaged 3 or 4 times maintained stem cell characteristics and can be used for DBP analysis. Two regulated DBPs, monobromoacetic acid(BAA) and monochloroacetic acid(CAA), and two emerging DBPs, 2,6-dibromo-1,4-benzoquinone(2,6-DBBQ) and 2,6-dichloro-1,4-benzoquinone(2,6-DCBQ), were chosen for h NSC treatment. Both 2,6-DBBQ and 2,6-DCBQ induced cell cycle arrest at S-phase at concentrations up to 1 μmol/L. Comparatively, BAA and CAA at 0.5 μmol/L affected neural differentiation. These results suggest DBP-dependent effects on h NSC proliferation and differentiation. The DBP-induced cell cycle arrest and inhibition of normal h NSC differentiation demonstrate the need to assess the developmental neurotoxicity of DBPs.
文摘When bromide/iodide is present in source water, hypobromous acid/hypoiodous acid will be formed with addition of chlorine, chloramine, or other disinfectants. Hypobromous acid/hypoiodous acid undergoes reactions with natural organic matter in source water to form numerous brominated/iodinated disinfection byproducts (DBPs). In this study, tap water samples were collected from eight cities in China. With the aid of electrospray ionization-triple quadrupole mass spectrometry by setting precursor ion scans of m/z 35, m/z 81, and m/z 126.9, whole pictures of polar chlorinated, brominated, and iodinated DBPs in the tap water samples were revealed for the first time. Numerous polar halogenated DBPs were detected, including haloacetic acids, newly identified halogenated phenols, and many new/unknown halogenated compounds. Total organic chlorine, total organic bromine, and total organic iodine were also measured to indicate the total levels of all chlorinated, brominated, and iodinated DBPs in the tap water samples. The total organic chlorine concentrations ranged from 26.8 to 194.0 μg· L 1 as Cl, with an average of 109.2 μg·L-1 as Cl; the total organic bromine concentrations ranged from below detection limit to 113.3 μg·L-1 as Br, with an average of 34.7 μg·L-1 as Br; the total organic iodine concentrations ranged from below detection limit to 16.4 μg· L-1 as I, with an average of 9.1 μg· L-1 as I; the total organic halogen concentrations ranged from 31.3 to 220.4 μg·L-1 as Cl, with an average of 127.2 μg· L- 1 as Cl.
基金supported by the National Science Foundation (No. 1833108)。
文摘In the race to deliver clean water to communities through potable water reuse, disinfection and water quality assessment are and will continue to be fundamental factors. There are over 700 disinfection byproducts(DBPs) in water;evaluating each compound is practically impossible and very time consuming. A bioanalytical approach could be an answer to this challenge. In this work, the response of four major classes of DBPs toward mitochondrial membrane potential( Δψm) and cytoplasmic adenosine triphosphate(C-ATP) was investigated with human carcinoma(Hep G2) cells. Within 90 min of cell exposure, only the haloacetic acid(HAA) mixture caused a cytotoxic response as measured by C-ATP. All four groups(haloacetonitriles(HANs), trihalomethanes(THMs), nitrosamines(NOAs), and HAAs) responded well to Δψm, R 2 > 0.70. Based on the half-maximum concentration that evoked a 50% response in Δψm, the response gradient was HANs >> HAAs ~ THM > NOAs. The inhibition of the Δψm by HANs is driven by dibromoacetonitrile(DBAN), while dichloroacetonitrile(DCAN) did not cause a significant change in the Δψm at less than 2000 μM. A mixture of HANs exhibited an antagonistic behavior on the Δψm compared to individual compounds. If water samples are concentrated to increase HAN concentrations, especially DBAN, then Δψm could be used as a biomonitoring tool for DBP toxicity.
基金supported by the National Natural Science Foundation of China(Nos.22176089 and 52270072)funding from the State Key Laboratory of Pollution Control and Resource Reuse(China)(No.PCRR-ZZ-202103).
文摘Disinfection byproducts (DBPs) are emerging pollutants in drinking water with high health risks. Precursor reduction before disinfection is an effective strategy to control the formation of DBPs. In this study, three types of anion exchange resins (AERs) and two types of nanofiltration (NF) membranes were tested for their control effects on DBP precursors, DBPs, and total organic halogen (TOX). The results showed that, for AER adsorption, the removal efficiencies of DBP precursors, DBPs, and TOX increased with the increase of resin dose, and the strong basic macroporous anion exchange resin (M500MB) had the highest removal efficiencies. For NF, the highest removal efficiencies were achieved at an operating pressure of 4 bar, and the membrane (NF90) with a smaller molecular weight cut-off, had a better control efficiency. However, AER adsorption was inefficient in removing dissolved organic carbon (DOC);NF was inefficient in removing Br− resulting in insufficient control of Br-DBPs. Accordingly, a sequential approach of AER (M500MB) adsorption followed by NF (NF90) was developed to enhance the control efficiency of DBPs. Compared with single AER adsorption and single NF, the sequential approach further increased the removal efficiencies of DOC by 19.4%–101.9%, coupled with the high Br− removal efficiency of 92%, and thus improved the reduction of cyclic DBPs and TOX by 3.5%–4.9%, and 2.4%–8.4%, respectively;the sequential approach also reduced the cytotoxicity of the water sample by 66.4%.
基金supported by grants from the Natural Sciences and Engineering Research Council of Canada,Alberta Health,and Alberta Innovates-Energy and Environment Solutions
文摘A broad range of organic compounds are known to exist in drinking water sources and serve as precursors of disinfection byproducts(DBPs).Epidemiological findings of an association of increased risk of bladder cancer with the consumption of chlorinated water has resulted in health concerns about DBPs.Peptides are thought to be an important category of DBP precursors in water.However,little is known about the actual presence of peptides and their DBPs in drinking water because of their high sample complexity and low concentrations.To address this challenge and identify peptides and non-chlorinated/chlorinated peptide DBPs from large sets of organic compounds in water,we developed a novel high throughput analysis strategy,which integrated multiple solid phase extraction(SPE),high performance liquid chromatography(HPLC)separation,and non-target identification using precursor ion exclusion(PIE)high resolution mass spectrometry(MS).After MS analysis,structures of candidate compounds,particularly peptides,were obtained by searching against the Human Metabolome Database(HMDB).Using this strategy,we successfully detected 625 peptides(out of 17,205 putative compounds)and 617 peptides(out of 13,297)respectively in source and finished water samples.The source and finished water samples had 501 peptides and amino acids in common.The remaining 116 peptides and amino acids were unique to the finished water.From a subset of 30 putative compounds for which standards were available,25 were confirmed using HPLC-MS analysis.By analyzing the peptides identified in source and finished water,we successfully confirmed three disinfection reaction pathways that convert peptides into toxic DBPs.
基金supported by the National Natural Science Foundation of China (No. 21876210)。
文摘Chlorine, chlorine dioxide, and ozone are widely used as disinfectants in drinking water treatments. However, the combined use of different disinfectants can result in the formation of various organic and inorganic disinfection byproducts(DBPs). The toxic interactions, including synergism, addition, and antagonism, among the complex DBPs are still unclear. In this study, we established and verified a real-time cell analysis(RTCA) method for cytotoxicity measurement on Chinese hamster ovary(CHO) cell. Using this convenient and accurate method, we assessed the cytotoxicity of a series of binary combinations consisting of one of the 3 inorganic DBPs(chlorite, chlorate, and bromate) and one of the 32 regulated and emerging organic DBPs. The combination index(CI) of each combination was calculated and evaluated by isobolographic analysis to reflect the toxic interactions. The results confirmed the synergistic effect on cytotoxicity in the binary combinations consisting of chlorite and one of the 5 organic DBPs(2 iodinated DBPs(I-DBPs) and 3 brominated DBPs(Br-DBPs)), chlorate and one of the 4 organic DBPs(3 aromatic DBPs and dibromoacetonitrile), and bromate and one of the 3 organic DBPs(2 I-DBPs and dibromoacetic acid). The possible synergism mechanism of organic DBPs on the inorganic ones may be attributed to the influence of organic DBPs on cell membrane and cell antioxidant system. This study revealed the toxic interactions among organic and inorganic DBPs, and emphasized the latent adverse outcomes in the combined use of different disinfectants.
基金funding from the National Science Foundation (No. CBET 1705206)the University of South Carolina, and the Chinese Scholarship Council (No. CSC 201908350069)。
文摘Halogenated disinfection byproducts(DBPs) are an unintended consequence of drinking water disinfection, and can have significant toxicity. XAD resins are commonly used to extract and enrich trace levels of DBPs for comprehensive, nontarget identification of DBPs and also for in vitro toxicity studies. However, XAD resin recoveries for complete classes of halogenated DBPs have not been evaluated, particularly for low, environmentally relevant levels(ng/L to low μg/L). Thus, it is not known whether levels of DBPs or the toxicity of drinking water might be underestimated. In this study, DAX-8/XAD-2 layered resins were evaluated, considering both adsorption and elution from the resins, for extracting 66 DBPs from water. Results demonstrate that among the 7 classes of DBPs investigated, trihalomethanes(THMs), including iodo-THMs, were the most efficiently adsorbed, with recovery of most THMs ranging from 50%-96%, followed by halonitromethanes(40%-90%). The adsorption ability of XAD resins for haloacetonitriles, haloacetamides, and haloacetaldehydes was highly dependent on the individual species. The adsorption capacity of XAD resins for haloacetic acids was lower(5%-48%), even after adjusting to p H 1 before extraction. Recovery efficiency for most DBPs was comparable with their adsorption, as most were eluted effectively from XAD resins by ethyl acetate. DBP polarity and molecular weight were the two most important factors that determine their recovery. Recovery of trichloromethane, iodoacetic acid, chloro-and iodo-acetonitrile, and chloroacetamide were among the lowest, which could lead to underestimation of toxicity, particularly for iodoacetic acid and iodo-acetonitrile, which are highly toxic.