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1.
Chlorine disinfection of secondary wastewater effluent and drinking water can result in the production of the potent carcinogen N-nitrosodimethylamine (NDMA) at concentrations of approximately 100 and 10 parts per trillion (ng/L), respectively. Laboratory experiments with potential NDMA precursors indicate that NDMA formation can form during the chlorination of dimethylamine and other secondary amines. The formation of NDMA during chlorination may involve the slow formation of 1,1-dimethylhydrazine by the reaction of monochloramine and dimethylamine followed by its rapid oxidation to NDMA and other products including dimethylcyanamide and dimethylformamide. Other pathways also lead to NDMA formation during chlorination such as the reaction of sodium hypochlorite with dimethylamine. However, the rate of NDMA formation is approximately an order of magnitude slower than that observed when monochloramine reacts with dimethylamine. The reaction exhibits a strong pH dependence due to competing reactions. It may be possible to reduce NDMA formation during chlorination by removing ammonia prior to chlorination, by breakpoint chlorination, or by avoidance of the use of monochloramine for drinking water disinfection. 相似文献
2.
N-nitrosodimethylamine (NDMA)formation in chloraminated Iowa River water (IRW) is primarily attributed to reactions with natural organic matter (NOM) generally classified as humic substances. Experiments were conducted to determine the contribution of various NOM humic fractions to the NDMA formation potential (NDMA FP) in this drinking water source. NOM was concentrated by reverse osmosis (RO) and humic fractions were obtained by a series of resin elution procedures. Mass balances showed that nearly 90% of the NDMA formation potential could be recovered in the NOM concentrate and in water reconstituted using additions of the various humic fractions. Generally, the hydrophilic fractions tended to form more NDMA than hydrophobic fractions, and basic fractions tend to form more NDMA than acid fractions when normalized to a carbon basis. Overall, the hydrophobic acid fraction was the dominant source of NDMA when both formation efficiency and water composition were considered. The amount of NDMA formed in a sample was found to correlate linearly with an oxidation-induced decrease in specific UV absorbance (SUVA) value at 272 nm. This is consistent with a mechanism in which precursors are formed as the direct consequence of the oxidation of NOM. The NDMA FP estimated using the slope of this relationship and the initial SUVA value compared closely to the value obtained by measuring the NDMA formed in solutions dosed with excess concentrations of monochloramine that presumably exhaust all potential precursor sources. However, the NOMA FP could not be correlated to the SUVA value of the individual humic fractions indicating that the relationship of the NDMA FP to SUVA value is probably a water-specific parameter dependent on the exact composition of humic fractions. It is hypothesized that either specific NDMA precursors are distributed among the various humic fractions or that the humic material itself represents a "generic" nonspecific precursor source that requires some degree of oxidation to eventually produce NDMA. The nonmonotonic behavior of NOM fluorescence spectra during chloramination and lack of correlation between NOM fluorescence characteristics and NDMA formation limited the usage of fluorescence spectra into probing NDMA formation. 相似文献
3.
Photochemical attenuation of N-nitrosodimethylamine (NDMA) and other nitrosamines in surface water 总被引:2,自引:0,他引:2
The aqueous photolysis of seven alkyl nitrosamines was studied by irradiation in a solar simulator. Nitrosamines included N-nitrosodimethylamine (NDMA), N-nitrosomethylethylamine (NMEA), N-nitrosodiethylamine (NDEA), N-nitrosodi-n-propylamine (NDPA), N-nitrosodi-n-butylamine (NDBA), N-nitrosopiperidine (NPip), and N-nitrosopyrrolidine (NPyr). Direct photolysis at irradiations of 765 W/m2, representing Southern California midsummer, midday sun, resulted in half-lives of 16 min for NDMA and 12-15 min for the other nitrosamines. The quantum yield for NDMA was determined to be phi = 0.41 and phi = 0.43-0.61 for the other nitrosamines. Quantified products of NDMA photolysis included methylamine, dimethylamine, nitrite, nitrate, and formate, with nitrogen and carbon balances exceeding 98 and 79%, respectively. Indirect photolysis of nitrosamines in surface water was not observed; increasing dissolved organic carbon (DOC) slowed the NDMA photolysis rate because of light screening. Removal of NDMA measured in tertiary treated effluent flowing in a shallow, sunlit engineered channel agreed with photolysis rates predicted based on the measured quantum yield and system parameters. Because biodegradation is relatively slow, aquatic photolysis of NDMA is generally expected to be more significant even at relatively low levels of solar irradiation (t(1/2) = 8-38 h at 244-855 W/m2, 51 degrees N latitude, 1 m depth). 相似文献
4.
The oxidation of N-nitrosodimethylamine (NDMA) precursors chlorine dioxide (ClO2). Second-order rate constants for the reactions of model NDMA precursors (dimethylamine (DMA) and 7 tertiary amines) with ozone (kapp at pH 7 = 2.4 x 10(-1) to 2.3 x 10(9) M(-1) s(-1)), ClO2 (kapp at pH 7 = 6.7 x 10(-3) to 3.0 x 10(7) M(-1) s(-1)), and hydroxyl radical (*OH) (kapp at pH 7 = 6.2 x 10(7) to 1.4 x 10(10) M(-1) s(-1)) were determined, which showed that the selected NDMA precursors, with the exception of dimethylformamide (DMFA) can be completely transformed via their direct reaction with ozone. During ozonation, DMFA may be partially transformed through oxidation by the secondary oxidant *OH. ClO2 was also shown to effectively transform most of the precursors, with the exceptions of DMA and DMFA. In the second part of the study, the NDMA formation potentials (NDMA-FP) in synthetic and natural waters were measured with and without pre-oxidation with ozone and ClO2. A significant reduction in the NDMA-FPs was observed after complete transformation of the model NDMA precursors. Ozonation generally led to more effective reduction of the NDMA-FP than ClO2. For most of the precursors, the formation of DMA could account for the NDMA-FPs remaining after complete transformation of the model NDMA precursors. In contrast, dimethylethanolamine and dimethyldithiocarbamate yielded other NDMA precursors (not DMA) as their oxidation products. Pre-oxidation by ozone and ClO2 of several natural waters showed behavior similar to that of the oxidation of model NDMA precursors with a reduction of the NDMA-FP by 32-94% for various natural water sources. 相似文献
5.
The uptake and fate of the emerging contaminants N-nitrosodimethylamine (NDMA) and perchlorate in phreatophytes was studied in a hydroponics system under greenhouse conditions. NDMA is a potent carcinogen, and perchlorate disrupts the functioning ofthe human thyroid gland. The rate of removal of NDMA from solution by rooted cuttings of black willow (Salix nigra) and hybrid poplar (Populus deltoides x nigra, DN34) trees varied seasonally, with faster removal in summer months when transpiration rates were highest. A linear correlation between the volume of water transpired and mass of NDMA removed from the root zone was observed, especially at higher NDMA concentrations. In bioreactors dosed with both NDMA (0.7-1.0 mg L(-1)) and perchlorate (27 mg L(-1)), no competitive uptake of NDMA and perchlorate was observed. While NDMA was primarily removed from solution by plant uptake, perchlorate was predominantly removed by rhizodegradation. In the presence of NDMA, a slower rate of rhizodegradation of perchlorate was observed, but still significantly faster than the rate of NDMA uptake. For experiments conducted with radiolabeled NDMA, 46.4 +/- 1.1% of the total 14C-activity was recovered in the plant tissues and 47.5% was phytovolatilized. The 46.4 +/- 1.1% recovered in the plants was distributed as follows: 18.8 +/- 1.4% in leaves, 15.9 +/- 5.9% in stems, 7.6 +/- 3.2% in branches, and 3.5 +/- 3.3% in roots. The poor extractability of NDMA with methanol-water (1:1 v/v) from stem and leaf tissues suggested that some fraction of NDMA was assimilated. The calculated transpiration stream concentration factor (TSCF) of 0.28 +/- 0.06 suggests that NDMA is passively taken up by phreatophytes, and mainly phytovolatilized. 相似文献
6.
The influence of the pre-oxidation of natural organic matter on the formation of N-nitrosodimethylamine (NDMA) 总被引:1,自引:0,他引:1
NDMA is a recently recognized disinfection byproduct that can be formed by a reaction of monochloramine with natural organic matter (NOM). This study was undertaken to examine the influence of various preoxidation strategies (including prechlorination) on the subsequent formation of NDMA and to determine how this is correlated to the subsequent loss in specific UV absorbance (SUVA) that preoxidation causes. Batch experiments were conducted using surface-water-derived NOM exposed to various oxidants that included free chlorine, permanganate, hydrogen peroxide, and ozone. Photochemical oxidation was also studied by exposing the water to simulated sunlight The amount of NDMA formed after monochloramine was added or formed in situ, in the case when free chlorine was the preoxidant, was significantly reduced by these treatments. The reduction was proportional to the reduction in SUVA that also occurred as a consequence of these treatments indicating that SUVA may be a good surrogate for NDMA precursor content. Furthermore, the change in NDMA formation per unit change in SUVA was a constant that did not depend on the nature of the oxidant 相似文献
7.
Modeling the formation of N-nitrosodimethylamine (NDMA) from the reaction of natural organic matter (NOM) with monochloramine 总被引:2,自引:0,他引:2
This paper presents mechanistic studies on the formation of NDMA, a newly identified chloramination disinfection byproduct, from reactions of monochloramine with natural organic matter. A kinetic model was developed to validate proposed reactions and to predict NDMA formation in chloraminated water during the time frame of 1-5 days. This involved incorporating NDMA formation reactions into an established comprehensive model describing the oxidation of humic-type natural organic matter by monochloramine. A rate-limiting step involving the oxidation of NOM is theorized to control the rate of NDMA formation which is assumed to be proportional to the rate of NOM oxidized by monochloramine. The applicability of the model to describe NDMA formation in the presence of three NOM sources over a wide range in water quality (i.e., pH, DOC, and ammonia concentrations) was evaluated. Results show that with accurate measurement of monochloramine demand for a specific supply, NDMA formation could be modeled over an extended range of experimental conditions by considering a single NOM source-specific value of thetaNDMA, a stoichiometric coefficient relating the amount of NDMA produced to the amount of NOM oxidized, and several kinetic parameters describing NOM oxidation. Furthermore, the oxidation of NOM is the rate-limiting step governing NDMA formation. This suggests that NDMA formation over a 1-5 day time frame may be estimated from information on the chloramine or free chlorine demand of the NOM and the source-specific linear relationship between this demand and NDMA formation. Although the proposed model has not yet been validated for shorter time periods that may better characterize the residence time in some distribution systems, the improved understanding of the important reactions governing NDMA formation and the resulting model should benefit the water treatment industry as a tool in developing strategies that minimize NDMA formation. 相似文献
8.
Padhye L Luzinova Y Cho M Mizaikoff B Kim JH Huang CH 《Environmental science & technology》2011,45(10):4353-4359
Interactions of ozone with organic precursors during water treatment may generate carcinogenic N-nitrosodimethylamine (NDMA) byproduct. This study investigates the reaction mechanisms responsible for NDMA formation from ozonation of the commonly used poly(diallyldimethylammonium chloride) (polyDADMAC) coagulant. Upon ozonation, polyDADMAC yields the highest amount of NDMA among several water treatment polymers, including polyamines and cationic polyacrylamides. Ozonation transforms polyDADMAC to dimethylamine (DMA) and NDMA formation is correlated to polyDADMAC degradation and DMA release. Hydroxyl radicals generated from ozone play an important role in the degradation of polyDADMAC's quaternary ammonium ring groups and subsequent release of secondary amine. Although nitrite and formaldehyde are detected as ozonation products of DMA and polyDADMAC, contribution of formaldehyde-enhanced nitrosation pathway is determined to be insignificant in NDMA formation. In contrast, reaction of hydroxylamine, another ozonation product of DMA, with DMA in the presence of ozone is deemed critical in the formation of NDMA during ozonation. The study results show that that contact of polyDADMAC with ozone will lead to release of the more potent NDMA precursor DMA but may not generate a significant amount of NDMA under typical drinking water treatment conditions due to low yield. The mechanistic understanding from this study can help develop source control strategies for minimization of NDMA formation risk at water and wastewater utilities. 相似文献
9.
Oxidation kinetics of selected taste and odor compounds during ozonation of drinking water 总被引:6,自引:0,他引:6
The applicability of ozonation to mitigate taste and odor problems in drinking water was investigated. Second-order rate constants of eleven taste and odor compounds with ozone and hydroxyl radicals were determined under laboratory conditions. Measured rate constants for the reaction with hydroxyl radicals are between 3 x 10(9) and 10(10) M(-1)s(-1) and for ozone: kbeta-cyclocitral = 3890 +/- 140 M(-1)s(-1); kgeosmin = 0.10 +/- 0.03 M(-1)s(-1); k3-hexen-1-ol = 5.4 +/- 0.5 x 10(5) M(-1)s(-1); kbeta-ionone = 1.6 +/- 0.13 x 10(5) M(-1)s(-1); k2-isopropyl-3-methoxypyrazine = 50 +/- 3 M(-1)s(-1); k2-methylisoborneol = 0.35 +/- 0.06 M(-1)s(-1); k2,6-nonadienal = 8.7 +/- 0.4 x 10(5) M(-1)s(-1); k1-penten-3-one = 5.9 +/- 0.1 x 10(4) M(-1)s(-1); k2,6-di-tert-butyl-4-methylphenol (BHT) = 7.4 +/- 0.2 x 10(4) M(-1)s(-1); k2,4,6-tribromoanisole = 0.02 +/- 0.01 M(-1)s(-1); k2,4,6-trichloroanisole = 0.06 +/- 0.01 M(-1)s(-1). Experiments conducted in natural waters showed that the removal efficiency during ozonation can be reliably predicted with the determined second-order rate constants. Ozonation is a powerful tool capable of oxidizing most of the taste and odor compounds to more than 50% under typical drinking water treatment conditions. For ozone-resistant taste and odor compounds, the application of advanced oxidation processes may be appropriate. 相似文献
10.
Dissolved organic nitrogen as a precursor for chloroform, dichloroacetonitrile, N-nitrosodimethylamine, and trichloronitromethane 总被引:7,自引:0,他引:7
Nitrogen-containing disinfection byproducts (N-DBPs) are potentially toxic. This study assessed the formation of three N-DBPs (dichloroacetonitrile (DCAN), trichloronitromethane (TCNM), and N-nitrosodimethylamine (NDMA)) and one regulated DBP (chloroform) upon adding free chlorine and monochloramine into solutions containing different fractions (hydrophobic, transphilic, hydrophilic, and colloidal) of dissolved organic matter (DOM) isolates (n=17). We hypothesized that N-DBP formation would increase for organic matter enriched in organic nitrogen. Formation potential tests were conducted with free chlorine or preformed monochloramine. Chloramination formed, on average, 10 times lower chloroform concentrations, but 5 times higher DCAN concentrations, as compared with free chlorine addition. The formation of the two halogenated N-DBPs (DCAN and TCNM) increased as the dissolved organic carbon (DOC) to dissolved organic nitrogen (DON) ratio decreased upon adding free chlorine, but the N-DBP formation was relatively constant upon adding monochloramine. NDMA, a nonhalogenated N-DBP, formed on average 0.26 nmol per mg of DOC (4.5 nmol per mg of DON) upon adding monochloramine; no NDMA formation occurred upon adding free chlorine. NDMA formation increased as the DOC/DON ratio decreased (i.e., increasing nitrogen content of DOM). NDMA formation also increased as the amino sugar to aromatic ratio of DOM increased. The results support the hypothesis that DON promotes the formation of N-DBPs. 相似文献
11.
Fabrication of catalytic membranes for the treatment of drinking water using combined ozonation and ultrafiltration 总被引:1,自引:0,他引:1
The removal of disinfection byproducts and their precursors was investigated using a combined ozonation-ultrafiltration system. A commercial membrane was coated 20 or 40 times with iron oxide nanoparticles (4-6 nm in diameter). With this membrane, the concentration of dissolved organic carbon was reduced by >85% and the concentrations of simulated distribution system total trihalomethanes and simulated distribution system halo acetic acids decreased by up to 90% and 85%, respectively. When the coated membrane was used, the concentrations of aldehydes, ketones, and ketoacids in the permeate were reduced by >50% as compared to that obtained with the uncoated membranes. Hydroxyl or other radicals produced at the iron oxide coated membrane surface as a result of ozone decomposition are believed to have enhanced the degradation of the natural organic matter, thereby reducing the concentration of disinfection byproducts. While increasing the number of times the membrane was coated from 20 to 40 did not significantly reduce the concentrations of most of the parameters measured, it did result in a significant decrease in the concentrations of ozonation byproducts. Increasing the sintering temperature from 500 to 900 degrees C also resulted in an improvement in the removal of the ozonation byproducts. 相似文献
12.
Delaney MF Blodget C Hoey CE McSweeney NE Epelman PA Rhode SF 《Environmental science & technology》2007,41(24):8383-8387
Carefully controlled bench-scale and on-site experiments demonstrated that cyanide can form in the treated drinking water sample container during preservation and storage. In the bench-scale experiment, treated tap water samples were collected on 20 days over six months. The tap water samples were split and some of the splits were spiked with formaldehyde, a known ozone disinfection byproduct, held for three hours and tested for cyanide. Then they were preserved and held for 2-10 days. None of the 69 initial samples had cyanide detects, but 22 of 49 formaldehyde-spiked samples and three of the 20 unspiked samples developed detectable cyanide concentrations during storage. In the on-site experiment, six samples were collected at a finished water tap at an ozone/chloramination treatment plant over three days. Each sample was split, and a portion was spiked with formaldehyde. Each portion was analyzed in triplicate after three different procedures: (1) immediately distilled on-site, (2) stabilized on-site in a distillation tube and distilled back at the laboratory several days later, or (3) following the conventional procedure of preserving the sample to pH > 12 in a container and distilling the sample back at the laboratory. Only the samples handled in the conventional way had detectable amounts of cyanide. Both experiments demonstrated that cyanide can form during conventional preservation and storage, and it is likely that the cyanide detected for this treated drinking water was formed in the sample container as a consequence of the preservation and storage conditions. 相似文献
13.
Emergency drinking water treatment during source water pollution accidents in China: origin analysis, framework and technologies 总被引:5,自引:0,他引:5
China has suffered frequent source water contamination accidents in the past decade, which has resulted in severe consequences to the water supply of millions of residents. The origins of typical cases of contamination are discussed in this paper as well as the emergency response to these accidents. In general, excessive pursuit of rapid industrialization and the unreasonable location of factories are responsible for the increasing frequency of accidental pollution events. Moreover, insufficient attention to environmental protection and rudimentary emergency response capability has exacerbated the consequences of such accidents. These environmental accidents triggered or accelerated the promulgation of stricter environmental protection policy and the shift from economic development mode to a more sustainable direction, which should be regarded as the turning point of environmental protection in China. To guarantee water security, China is trying to establish a rapid and effective emergency response framework, build up the capability of early accident detection, and develop efficient technologies to remove contaminants from water. 相似文献
14.
Evrim Özkaynak Kanmaz 《Food science and biotechnology》2018,27(4):981-986
The aim of this study was to investigate the effect of material type (artichoke leave, lemon peel, flaxseed meal), extraction temperature (50, 100, 120, 140, 160, 180, 200 °C) and static extraction time (5, 15, 30, 45 min) on 5-hydroxymethylfurfural (5-HMF) formation during subcritical water extraction. 5-HMF content of artichoke leave and lemon peel extracts increased 7.2 and 26.1 times with the rise of extraction temperature from 160 to 180 °C for 5 min during subcritical water extraction, respectively. Besides, 5-HMF content of artichoke leave, lemon peel and flaxseed meal extracts increased 1.4, 2.0 and 4.5 times as static extraction time increased from 15 to 45 min at 180 °C during subcritical water extraction, respectively. The highest 5-HMF content of artichoke leave and lemon peel extracts were obtained as 58.83 and 231.21 mg/L at 180 °C and 45 min, respectively. However, for flaxseed meal, the highest 5-HMF content (222.94 mg/L) was obtained at 200 °C and 15 min during subcritical water extraction. 相似文献
15.
Fate of endocrine-disruptor, pharmaceutical, and personal care product chemicals during simulated drinking water treatment processes 总被引:24,自引:0,他引:24
The potential occurrence of endocrine-disrupting compounds (EDCs) as well as pharmaceuticals and personal care products (PPCPs) in drinking water supplies raises concern over the removal of these compounds by common drinking water treatment processes. Three drinking water supplies were spiked with 10 to 250 ng/L of 62 different EDC/ PPCPs; one model water containing an NOM isolate was spiked with 49 different EDC/PPCPs. Compounds were detected by LC/MS/MS or GC/MS/MS. These test waters were subjected to bench-scale experimentation to simulate individual treatment processes in a water treatment plant (WTP). Aluminum sulfate and ferric chloride coagulants or chemical lime softening removed some polyaromatic hydrocarbons (PAHs) but removed <25% of most other EDC/ PPCPs. Addition of 5 mg/L of powder activated carbon (PAC) with a 4-h contact time removed 50% to >98% of GC/ MS/MS compounds (more volatile) and 10% to >95% of LC/ MS/MS compounds (more polar); higher PAC dosages improved EDC/PPCP removal. EDC/PPCP percentage removal was independent of the initial compound concentration. Octanol-water partition coefficients served as a reasonable indicator of compound removal under controlled PAC test conditions, except for EDC/PPCPs that were protonated or deprotonated at the test pH and some that contained heterocyclic or aromatic nitrogen. Separate chlorine or ozone experiments decreased the EDC/PPCP initial concentration by <10% to >90%; EDC/PPCPs were likely transformed to oxidation byproducts. Ozone oxidized steroids containing phenolic moieties (estradiol, ethynylestradiol, or estrone) more efficiently than those without aromatic or phenolic moieties (androstenedione, progesterone, and testosterone). EDC/PPCP reactivity with oxidants were separated into three general groups: (1) compounds easily oxidized (>80% reacted) by chlorine are always oxidized at least as efficiently by ozone; (2) 6 of the -60 compounds (TCEP, BHC, chlordane, dieldrin, heptachlor epoxide, musk ketone) were poorly oxidized (<20% reacted) by chlorine or ozone; (3) compounds (24 of 60) reacting preferentially (higher removals) with ozone rather than chlorine. Conventional treatment (coagulation plus chlorination) would have low removal of many EDC/PPCPs, while addition of PAC and/or ozone could substantially improve their removals. Existing strategies that predict relative removals of herbicides, pesticides, and other organic pollutants by activated carbon or oxidation can be directly applied for the removal of many EDC/PPCPs, but these strategies need to be modified to account for charged (protonated bases or deprotonated acids) and aliphatic species. Some compounds (e.g., DEET, ibuprofen, gemfibrozil) had low removals unless ozonation was used. Other compounds had low removals by all the WTP processes considered (atrazine, iopromide, meprobamate, TCEP), and removal processes capable of removing these types of compounds should be investigated. 相似文献
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Multiple lines of evidence for indicating factors associated with the sources, transport, and fate of chloroform and three other trihalomethanes (THMs) in untreated groundwater were revealed by evaluating low-level analytical results and logistic regression results for THMs. Samples of untreated groundwater from wells used for drinking water were collected from 1996-2007 from 2492 wells across the United States and analyzed for chloroform, bromodichloromethane, dibromochloromethane, and bromoform by a low-level analytical method implemented in April 1996. Using an assessment level of 0.02 μg/L, chloroform was detected in 36.5% of public-well samples and 17.6% of domestic-well samples, with most concentrations less than 1 μg/L. Brominated THMs occurred less frequently than chloroform but more frequently in public-well samples than domestic-well samples. For both public and domestic wells, THMs occurred most frequently in urban areas. Logistic regression analyses showed that the occurrence of THMs was related to nonpoint sources such as urban land use and to point sources like septic systems. The frequent occurrence and concentration distribution pattern of THMs, as well as their frequent co-occurrence with other organic compounds and nitrate, all known to have anthropogenic sources, and the positive associations between THM occurrence and dissolved oxygen and recharge indicate the recycling of water that contains THMs and other anthropogenic contaminants. 相似文献
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通过瓶(桶)装饮用纯净水微生物检测过程,指出对样品的取样、培养基的制备及其整个操作过程应注意事项,提高了微生物检测的准确度。 相似文献