Environmental Science-Water Research & Technology
·
2023
·Vol. 9
·期 4
·1231-1237
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IF 5
Run Zhou,Zhifei Xu,Yukang Wu,Li Yang,Xiuzhu Li,Yuanhua Meng,Pengfei Zhu,Lingcan Kong,Xinliang Ding
Human exposure to disinfection by-products (DBPs) primarily occurs through the consumption of drinking water. Haloacetamides (HAcAms) are an emerging class of nitrogenous DBPs with higher levels of cytotoxicity and genotoxicity compared to those of regulated DBPs. Detecting ultra-trace levels of HAcAms in drinking water remains challenging despite the availability of multiple detection methods. This paper reports the first use of ultra-performance liquid chromatography–mass spectrometry/mass spectrometry (UPLC-MS/MS) to quantify 13 HAcAms in drinking water without pretreatment. Results from the analysis of water samples collected from four cities in East China showed total HAcAm concentrations of 0.21–6.12 μg L−1, which were comparable to previously reported data from other countries. Further, 11 out of 13 HAcAms were detected in 60 water samples, with diHAcAms being the predominant subclass. DCAcAm and BCAcAm were the primary HAcAms targeted for detection and two Iodo-HAcAms were detected. The average total HAcAm concentration in water samples disinfected with chloramine was significantly higher than that in water samples disinfected with chlorine. Additionally, the total HAcAm concentrations in water samples from a treatment plant (WTP) using the ozone-biological activated carbon (ozone-BAC) process were lower than those in water samples from WTPs that did not use this treatment process. The results of this study have significant implications for monitoring water quality and protecting human health.
研究领域:
环境科学
·
公共卫生
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2022
·
IF 2.042
Zhen Zhou,Xing Zhang,Tong Zhang,Wen Ma,Xiaojun Fang
Haloacetamides (HAcAms) is ubiquitously found in drinking water, which exhibits strong cytotoxicity and genotoxicity compared with conventional disinfection byproducts (DBPs). Herein, the degradation of HAcAms containing dichloroacetamide (DCAcAm) and trichloroacetamide (TCAcAm) by UV/peroxymonosulfate (PMS) process was studied. Degradation kinetics of DCAcAm and TCAcAm conformed to the first-order model, and the corresponding reaction constants were 2.27 × 10−3 and 1.94 × 10−3 s−1, respectively. The degradation rate raised with the increment of PMS dosage. During the investigation of water matrices including Cl–, HCO3–, and humic acid (HA), HCO3– and HA inhibited the degradation process whereas the influence of Cl– on the degradation was negligible. As evidenced by trapping test, •OH played the crucial role in the degradation of HAcAms. During the UV/PMS process, dechlorination was the main process. TCAcAm could be oxidized to DCAcAm and acetamide, and further mineralized to Cl–, CO2, H2O, NO2–, and NO3–. Our results demonstrated that UV/PMS could be an effective technique to degrade HAcAms in dinking water.
研究领域:
环境科学
·
水处理
·
化学工程
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL TOXICOLOGY AND PHARMACOLOGY
·
2022
·
IF 5.785
Dong Li,Wen Cheng,Jiehui Ren,Lu Qin,Xing Zheng,Tian Wan,Min Wang
It is important to study the stress effects and mechanisms of haloacetamide (HAcAm) disinfection byproducts to reveal their health hazards. In this context, toxicological g was applied to evaluate the effects of four HAcAms, revealing the status of gene expression on Escherichia coli in different stress response types (oxidative, protein, membrane, general, DNA). This study revealed that the main toxic action modes of these HAcAms were general and membrane stresses by high-resolution, real-time gene expression profiling combined with clustering analysis. The results of time-gene evaluation showed that the presence of chloroacetamide (CAcAm) and bromoacetamide (BAcAm) generated more reactive oxygen species , thus activating oxidative stress . Trichloroacetamide (tCAcAm) induced altered expression of glutathione marker genes and membrane stress-related genes, and iodoacetamide (IAcAm) caused severe DNA damage by damaging DNA strands and individual nucleotides mainly through damage to nucleic acids and bases. Furthermore, quantitative structure-activity relationship (QSAR) modelling results indicated that the biological activities of HAcAms were related to their quantum chemical and topological properties.
研究领域:
毒理学
·
分子生物学
·
环境科学
·
基因组学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Shenghua Chen,Wenhai Chu,Hongbin Wei,Hongying Zhao,Bin Xu,Naiyun Gao,Daqiang Yin
Haloacetamides (HAcAms), a class of highly toxic nitrogenous disinfection by-products (N-DBPs), have been widely detected in drinking water . The control of DBPs is an important measure to ensure the safety of drinking water. Due to the presence of residual chlorine and organic compounds that failed to be effectively removed, HAcAms could be formed in the finished drinking water distribution systems. In the study, Cu/Fe bimetal with different molar ratios of Cu to Fe was synthesized. This study reported that Cu/Fe bimetal reduced trichloroacetamide (TCAcAm) to dichloroacetamide (DCAcAm) and monoacetamide (MCAcAm), and the reduction ability of Fe was greatly improved due to the incorporation of Cu. The optimal HAcAm removal was achieved when the molar ratio of Cu to Fe was 2.0%, Cu/Fe bimetal could reach complete degradation of TCAcAm within 1 h. With the increase of Cu/Fe bimetal dose or the decrease of solution pH, the reduction ability of Cu/Fe bimetal for HAcAm removal also increased. The calculated integrated toxicity values from HAcAms, which was used to reflect the comprehensive control effect of Cu/Fe bimetal for HAcAms, were also reduced with the decrease of solution pH and the increase of bimetal dose. The release of Cu 2+ was not detected during the whole treatment process, Cu/Fe bimetal may be an excellent material for controlling DBPs as the end – control methods in tap water.
研究领域:
环境科学
·
水处理工程
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Shunke Ding,Wenhai Chu,Stuart W. Krasner,Yun Yu,Chao Fang,Bin Xu,Naiyun Gao
Haloacetamides (HAMs), a group of nitrogenous disinfection byproducts (N-DBPs), can decompose to form corresponding intermediate products and other DBPs. The stability of ten different HAMs, including two chlorinated, five brominated, and three iodinated species was investigated with and without the presence of chlorine, chloramines, and reactive solutes such as quenching agents. The HAM basic hydrolysis and chlorination kinetics were well described by a second-order kinetics model, including first-order in HAM and hydroxide and first-order in HAM and hypochlorite, respectively, whereas the HAM neutral hydrolysis kinetic was first-order in HAM. Furthermore, HAMs decompose instantaneously when exposed to hypochlorite, which was almost two and nine orders of magnitude faster than HAM basic and neutral hydrolysis, respectively. In general, HAM hydrolysis and chlorination rates both increased with increasing pH and the number of halogens substituted on the methyl group. Moreover, chlorinated HAMs are more unstable than their brominated analogs, followed by the iodinated ones, due to the decrease in the electron-withdrawing inductive effect from chlorine to iodine atom. During hydrolysis, HAMs mainly directly decompose into the corresponding haloacetic acids (HAAs) via a nucleophilic reaction between the carbonyl carbon and hydroxide. For HAM chlorination reactions, hypochlorite reacts with HAMs to form the N -chloro-HAMs ( N -Cl-HAMs) via Cl + transfer from chlorine to the amide nitrogen. N -Cl-HAMs can further degrade to form HAAs via hypochlorous acid addition. In contrast, the reactions between chloramines and HAMs were found to be insignificant. Additionally, four common quenching agents, including sodium sulfite , sodium thiosulfate , ascorbic acid , and ammonium chloride , were demonstrated to expedite HAM degradation, whereas ammonium chloride was the least influential among the four. Taft linear free energy relationships were established for both HAM hydrolysis and chlorination reactions, based on which the hydrolysis and chlorination rate constants for three monohaloacetamides were estimated. The hydrolysis and chlorination rates of 13 HAMs decreased in the following order: TCAM > BDCAM > DBCAM > TBAM > DCAM > BCAM > DBAM > CIAM > BIAM > DIAM > MCAM > MBAM > MIAM (where C = chloro, B = bromo, I = iodo, T = tri, D = di, M = mono). Lastly, using the HAM kinetic model established in this study, HAM half-lifes in drinking water distribution systems can be predicted on the basis of pH and residual chlorine concentration.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Chao Fang,Stuart W. Krasner,Wenhai Chu,Shunke Ding,Tiantao Zhao,Naiyun Gao
Haloacetamides (HAMs), an emerging class of disinfection by-products, have received increasing attention due to their elevated cyto- and genotoxicity. However, only limited information is available regarding the iodinated analogues. This study investigated the formation and speciation of iodinated haloacetamides (I-HAMs) and their chlorinated/brominated analogues during the chloramination of bromide and/or iodide-containing waters and a model compound solution over various time periods. The rapid formation of diiodoacetamide (DIAM) was observed during chloramination of three simulated samples, whereas brominated (Br-HAMs) and chlorinated haloacetamides (Cl-HAMs) increased slowly with increasing reaction time. To further understand the differences in the formation of HAMs containing different halogens, experiments with the model compound asparagine in the presence/absence of iodide were conducted. Moreover, iodine utilisation factors and iodine incorporation factors were observed to increase significantly faster and were substantially higher than those of bromine. This implied that, compared with bromide, iodide has substantially greater potential to be transformed to the corresponding HAMs during chloramination, similar to that of other classes of DBPs. That is, I-HAMs formed faster than the other species investigated, including Cl-HAMs and Br-HAMs, in the early reaction stages (0–3 h). The effect of the bromide/iodide ratio (i.e., constant iodide, increasing bromide) on I-HAM formation was also examined. With increasing bromide/iodide ratio, the formation of Br-HAMs increased and dichloroacetamide decreased, but the formation of DIAM was largely unchanged. This was consistent with the constant level of iodide in spite of the increasing bromide. Chlorine and ammonia are applied separately during chloramination in water treatment , so the effect of pre-chlorination (before adding ammonia) on the formation and speciation of I-HAMs during in situ chloramination was also evaluated. Effective mitigation of DIAM formation with in situ chloramination was achieved, and the efficiency improved with increasing pre-chlorination time, where iodide was oxidised to iodate . The HAM-associated cytotoxicity was calculated to determine the change in toxicity at different reaction times, bromide/iodide ratios, and pre-chlorination times. A similar trend as the formation of I-HAMs was observed, which increased rapidly in the first 3 h, but decreased somewhat subsequently. When the bromide/iodide ratio and pre-chlorination time was increased, the calculated toxicity of the HAMs increased (due to more formation of Br-HAMs and less Cl-HAMs) and decreased (due to less DIAM formation), respectively.
研究领域:
环境科学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Jinxiu Lou,Feilong Dong,Huijie Lu,Shuangxi Fang,Xiangliang Pan
Disinfection byproducts (DBPs), such as haloacetamides (HAMs), have been associated with adverse health outcomes, including bladder cancer. The potential for DBPs to exacerbate cellular senescence, thereby linking exposure to health impacts, remains underexplored. In this study, MRC-5 cells were exposed to HAMs at concentrations of 2, 5, and 8 μg/L for 30 days to simulate long-term exposure to levels found in drinking water. All six tested HAMs significantly increased the cellular senescence degree and enriched the cellular senescence pathway at the proteomic-wide level. Specifically, HAMs upregulated microRNA-24 expression, which increased p16 mRNA levels and decreased p16 protein levels, thereby activating oncogene-induced senescence pathways. Additionally, HAMs were found to covalently bind to TNRC6A, activating the p53/p21 pathway. Principal component analysis highlighted the critical role of functional groups in activating senescence, and the interaction between HAMs and TNRC6A could extend to at least 27 other amide-containing DBPs. Prolonged exposure to HAMs at environmentally relevant levels notably exacerbates cellular senescence, shedding light on a commonly overlooked phenomenon. Given the widespread presence of DBPs in drinking water and their continuous exposure in humans, their role in cellular senescence represents an ongoing public health concern.
研究领域:
环境科学
·
毒理学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Huang Huang,Kai-Li Shao,Si-Yu Duan,Chu-Ying Zhong
The catalytic effect of copper corrosion products, including copper ions , cupric oxide, and cuprous oxide, on the formation of haloacetamides and haloacetonitriles during chlorination of natural organic matter (NOM), model nitrogenous precursors, and real water samples was investigated. During chlorination of NOM, the presence of these copper corrosion products facilitated chlorine decay, and enhanced the formation of dichloroacetonitrile (DCAN) and dichloroacetamide (DCAcAm) with enhancement ratios of 45–59% and 64–137% after 10 h contact time, respectively. Six amino acids were selected as nitrogenous NOM surrogates for chlorination, and the results show that the enhancement of DCAN and DCAcAm formation by copper corrosion products was only observed for slow reacting amino acids, including glutamine, glutamic acid, and phenylamine , suggesting that copper corrosion products may enhance DCAN and DCAcAm formation by catalyzing NOM portions that are relatively inefficient precursors. When bromide and copper corrosion products were present, the formation of dihaloacetonitriles (DHANs) and dihaloacetamides (DHAcAms) could be enhanced during chlorination of NOM, but the degrees of bromine substitution for DHANs and DHAcAms decreased. Although copper corrosion products facilitated DHAN and DHAcAm hydrolysis with the facilitation increasing as the halogens shifted from chlorine to bromine, increased DHAN and DHAcAm concentrations was observed during chlorination of real water samples in the presence of copper corrosion products, confirming that the copper corrosion products had a catalytic effect on DHAN and DHAcAm formation that exceeded their catalytic effect on DHAN and DHAcAm hydrolysis. This study provides basic knowledge of disinfectant residuals and the fate of haloacetonitriles and haloacetamides in drinking water distribution systems where copper is used, which will be helpful for the management of safe water distribution.
研究领域:
环境科学
·
水处理工程
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Shunke Ding,Feifei Wang,Wenhai Chu,Zhongqi Cao,Yang Pan,Naiyun Gao
The effective removal of haloacetamides (HAMs) as a group of emerging disinfection by-products is essential for drinking water safety. This study investigated the degradation of 10 HAMs, including chlorinated, brominated, and iodinated analogues, by sodium sulfite (S(IV)) and the mechanism behind it. The results indicated that all HAMs, excluding chlorinated HAMs, decomposed immediately when exposed to S(IV). The reductive dehalogenation kinetics were well described by a second-order kinetics model, first-order in S(IV) and first-order in HAMs. The degradation rates of HAMs increased with the increase of pH and they were positively correlated with sulfite concentration, indicating that the reaction of S(IV) with HAMs mainly depends on sulfite. The rank order and relative activity of the reaction of sulfite with HAMs depends on bimolecular nucleophilic substitution reaction reactivity. The order of the reductive dehalogenation rates of HAMs versus the substitution of halogen atoms was iodo- > bromo- >> chloro-. During reductive dehalogenation of HAMs by sulfite, the α-carbon bound to the amide group underwent nucleophilic attack at 180° to the leaving group (halide). As a consequence, the halide was pushed off the opposite side, generating a transition state pentacoordinate. The breaking of the C-X bond and the formation of the new C-S bond occurred simultaneously and HAM sulfonate formed as the immediate product. Results suggest that S(IV) can be used to degrade brominated and iodinated HAMs in drinking water and therefore should not be added as a quenching agent before HAM analysis to accurately determine the HAM concentrations produced during water disinfection .
研究领域:
环境科学
·
水处理工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yan Shen,Xiaochen Liu,Junling Li,Jingsi Chen,Jiafu Li
Haloacetamides (HAMs) is a class of highly toxic emerging nitrogenous disinfection byproducts (N-DBPs) in drinking water, however the factors influencing the formation of HAMs by amino acids remain incompletely understood. Besides, a quantitative data regarding how many HAMs in chlorinated drinking water can attribute to amino acids in source water is lacking. To address this gap, HAMs formation during chlorination for 20 amino acids with different side-chains was analyzed. HAMs yield of 20 common amino acids during chlorination was 0.04–132 μg/mg-C. For different side-chains in amino acids, carboxyl group exhibited the highest HAM’s yield at 65.9 μg/mg-C, followed by aromatic rings (10.2 μg/mg-C), and containing nitrogen (10.1 μg/mg-C), respectively. In contrast, hydroxyl groups, sulfur-containing amino acids and those with only hydrogen and alkyl groups showed the lowest HAM’s yield (<1 μg/mg-C). HAM yields of basic and neutral amino acids were lower than that of acidic amino acids. HAM yields of nonpolar amino acids were lower than polar amino acids. The HAM formation potentials of amino acids in source water during chlorination were 14.8–5138 ng/L, with an average of 576 ng/L. Aspartic acid, asparagine, and histidine accounted for as much as 97 % of the theoretical HAMs formation. The theoretical calculation found that amino acids in source water contribute about 3.2 % of HAMs in chlorinated drinking water, which is close to that of lab-controlled experiments (4.3 %), suggesting that the role of amino acids on HAMs in chlorinated drinking water is overvalued. Our study reveals the role of precursor’s side-chains on toxic DBP formation as well their potential contribution to drinking water DBPs.
研究领域:
环境健康学
·
水处理化学
·
毒理学
·
环境污染物
·
分子结构与活性关系
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Di Zhang,Feifei Wang,Youli Duan,Shenghua Chen,Aihong Zhang,Wenhai Chu
Disinfection by-products (DBPs) are associated with various adverse health effects. Diversiform advanced treatment processes have been applied for the control of DBPs, but DBPs can still be frequently detected in tap water . Tea-leaves can be made into popular beverage and is itself a porous bio-adsorbent. By simulating tea brewing process, this study evaluated the removal of DBPs from drinking water during the tea brewing process. Removal of four trihalomethanes (THMs) and four haloacetamides (HAMs) by different fermentation degree tea-leaves was investigated. Little DBPs were removed by unfermented and semi-fermented tea-leaves (i.e., Meitan turquoise bud and Dahongpao tea) with less than 5% removal of HAMs, whereas 40% HAMs can be removed by fermented tea (i.e., Jinjunmei tea and Shuixian tea). Tea soup is neutral and slightly acidic, so little DBP hydrolysis was observed under typical tea-leaf brewing process. DBPs were mainly removed by volatilization and adsorption during tea brewing. Removal difference caused by DBP volatilization is very small. The DBP removal difference of four kinds of tea-leaves may be caused by fermentation degree. The surface of unfermented Meitan turquoise bud had a smooth and regular morphology, whereas a rough, irregular, hollow and spongy surface of fermented tea (i.e., Jinjunmei and Shuixian tea) was observed. Generally, the higher the degree of tea fermentation, the more adsorption sites, and the more removal of DBPs. Finally, the model, which takes the DBP initial concentration, tea-leaf dose and brewing time into account, was established under the experimental conditions to predict the variation of DBP concentration during tea brewing, and suggestions for DBP removal were provided to reduce DBP exposure risk. The integrated toxic risk during tea brewing was also investigated, and about 30% integrated cytotoxicity and 26% genotoxicity was reduced during Jinjunmei and Shuixian tea-leaf brewing.
研究领域:
环境科学
·
公共卫生
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2017
·
IF 6.065
Shunke Ding,Wenhai Chu,Tom Bond,Qi Wang,Naiyun Gao,Bin Xu,Erdeng Du
The occurrence of pharmaceuticals and personal care products (PPCPs) in natural waters, which act as drinking water sources, raises concerns. Moreover, those compounds incompletely removed by treatment have the chance to form toxic disinfection byproducts (DBPs) during subsequent disinfection. In this study, acetaminophen (Apap), commonly used to treat pain and fever, was selected as a model PPCP. The formation of carbonaceous and nitrogenous DBPs, namely trihalomethanes, haloacetonitriles, and haloacetamides, during chlor(am)ination of Apap was investigated. Yields of chloroform (CF), dichloroacetonitrile (DCAN), dicholoacetamide (DCAcAm), and tricholoacetamide (TCAcAm), during chlorination were all higher than from chloramination. The yields of CF continuously increased over 48 h during both chlorination and chloramination. During chlorination, as the chlorine/Apap molar ratios increased from 1 to 20, CF yields increased from 0.33 ± 0.02% to 2.52 ± 0.15%, while the yields of DCAN, DCAcAm and TCAcAm all increased then decreased. In contrast, during chloramination, increased chloramine doses enhanced the formation of all DBPs. Acidic conditions favored nitrogenous DBP formation, regardless of chlorination or chloramination, whereas alkaline conditions enhanced CF formation. Two proposed formation mechanisms are presented. The analysed DBPs formed during chlorination were 2 orders of magnitude more genotoxic and cytotoxicity than those from chloramination.
研究领域:
环境科学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）