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1.
The formation of disinfection by-products (DBPs) from chlorination and monochloramination of treated drinking waters was determined. Samples were collected after treatment at 11 water treatment works but before exposure to chlorine or monochloramine. Formation potential tests were carried out to determine the DBPs formed by chlorination and monochloramination. DBPs measured were trihalomethanes (THMs), haloacetic acids (HAAs), halonitromethanes (HNMs), haloacetonitriles (HANs), haloaldehydes (HAs), haloketones (HKs) and iodo-THMs (i-THMs). All waters had the potential to form significant levels of all the DBPs measured. Compared to chlorine, monochloramination generally resulted in lower concentrations of DBPs with the exception of 1,1-dichloropropanone. The concentrations of THMs correlated well with the HAAs formed. The impact of bromine on the speciation of the DBPs was determined. The literature findings that higher bromide levels lead to higher concentrations of brominated DBPS were confirmed.  相似文献   

2.
Formation of nitrogenous disinfection by-products (N-DBPs) of cyanogen chloride (CNCl), dichloroacetonitrile (DCAN) and chloropicrin was evaluated during chloramination of several selected groups of nitrogenous organic (organic-N) compounds, including α-amino acids, amines, dipeptides, purines, and pyrimidines, The intermediates generated, reaction pathways, and nitrogen origin in N-DBPs were explored as well. CNCl was observed in chloramination of all tested organic-N compounds, with glycine giving the highest yields. DCAN was formed during chloramination of glutamic acid, cytosine, cysteine, and tryptophan. Chloramination of most organic-N compounds except for cysteine and glutamic acid generated chloropicrin. Aldehydes and nitriles were identified as the intermediates by negative mode electrospray ionization mass spectrometry during reactions of NH2Cl and organic-N compounds. Labeled 15N-monochloramine (15NH2Cl) techniques showed that nitrogen in N-DBPs may originate from both NH2Cl and organic-N compounds and the nitrogen partition percentages vary as functions of reactants and pH.  相似文献   

3.
Le Roux J  Gallard H  Croué JP 《Water research》2011,45(10):3164-3174
Disinfection with chloramines is often used to reduce the production of regulated disinfection by-products (DBPs) such as trihalomethanes (THMs) and haloacetic acids (HAAs). However, chloramination can lead to the formation of N-nitrosamines, including N-nitrosodimethylamine (NDMA), a probable human carcinogen. Previous research used dimethylamine (DMA) as a model precursor of NDMA, but certain widely used tertiary dimethylamines (e.g. the pharmaceutical ranitidine) show much higher conversion rates to NDMA than DMA. This study investigates the NDMA formation potential of several tertiary amines including pharmaceuticals and herbicides. The reactivity of these molecules with monochloramine (NH2Cl) is studied through the formation of NDMA, and other halogenated DBPs such as haloacetonitriles (HANs) and AOX (Adsorbable Organic Halides). Several compounds investigated formed NDMA in greater amounts than DMA, revealing the importance of structural characteristics of tertiary amines for NDMA formation. Among these compounds, the pharmaceutical ranitidine showed the highest molar conversion to NDMA. The pH and dissolved oxygen content of the solution were found to play a major role for the formation of NDMA from ranitidine. NDMA was formed in higher amounts at pH around pH 8 and a lower concentration of dissolved oxygen dramatically decreased NDMA yields. These findings seem to indicate that dichloramine (NHCl2) is not the major oxidant involved in the formation of NDMA from ranitidine, results in contradiction with the reaction mechanisms proposed in the literature. Dissolved oxygen was also found to influence the formation of other oxygen-containing DBPs (i.e. trichloronitromethane and haloketones). The results of this study identify several anthropogenic precursors of NDMA, indicating that chloramination of waters impacted by these tertiary amines could lead to the formation of significant amounts of NDMA and other non-regulated DBPs of potential health concern (e.g. dichloroacetonitrile or trichloronitromethane). This could be of particular importance for the chloramination of wastewater effluents, especially during water reuse processes.  相似文献   

4.
The use of population-level indices to estimate individual exposures is an important limitation of previous epidemiologic studies of disinfection by-products (DBPs). We examined exposure misclassification resulting from the use of system average DBP concentrations to estimate individual-level exposures. Data were simulated (n=1000 iterations) for 100 subjects across 10 water systems based on the following assumptions: DBP concentrations ranged from 0-99 microg/L with limited intra-system variability; water intake ranged from 0.5-2.5 L/day; 20% of subjects used bottled water exclusively; 20% of subjects used filtered tap water exclusively; DBP concentrations were reduced by 50% or 90% following filtration. DBP exposure percentiles were used to classify subjects into different exposure levels (e.g., low, intermediate, high and very high) for four classification approaches. Compared to estimates of DBP ingestion that considered daily consumption, source type (i.e., unfiltered tap, filtered tap, and bottled water), and filter efficiency (with 90% DBP removal), 48-62% of subjects were misclassified across one category based on system average concentrations. Average misclassification across at least two exposure categories (e.g., from high to low) ranged from 4-14%. The median classification strategy resulted in the least misclassification, and volume of water intake was the most influential modifier of ingestion exposures. These data illustrate the importance of individual water use information in minimizing exposure misclassification in epidemiologic studies of drinking water contaminants.  相似文献   

5.
Seven water treatment works were selected to compare disinfection by-products (DBPs) formed when using chlorination and chloramination. DBPs measured included trihalomethanes (THMs), haloacetic acids (HAAs), haloacetonitriles (HANs), trihalonitromethane, iodinated THMs and nitrosamines. Generally treatment works that used chloramination were able to meet the European THM regulatory limit of 100 μg L−1 whereas the chlorinated works found it significantly more difficult. There were no significant differences in the levels of nitrogenous DBPs between the treatment works using chlorination or chloramination with the exception of the nitrosamine N-nitrosodimethylamine (NDMA) which was present at one treatment works in one season.  相似文献   

6.
The effect of boiling water on disinfection by-product exposure   总被引:1,自引:0,他引:1  
Chloraminated and chlorinated waters containing bromide were used to determine the impact of boiling on disinfection by-product (DBP) concentrations. No significant changes were detected in the concentrations of the dihalogenated haloacetic acids (DXAAs) (i.e., dichloro-, bromochloro-, dibromoacetic acid) upon boiling of chloraminated water, whereas the levels of the trihalogenated haloacetic acids (TXAAs) (i.e., trichloro- (TCAA), bromodichloro- (BDCAA), dibromochloroacetic acid (DBCAA)) decreased over time (e.g., 9-37% for TCAA). Increased DXAA concentrations (58-68%) were detected in the boiled chlorinated sample, which likely resulted from residual chlorine reacting with DXAA precursors. TCAA concentration was unchanged after boiling chlorinated water for 1 min, but a 30% reduction was observed after 5 min of boiling. BDCAA concentrations decreased 57% upon boiling for 1 min and were completely removed after 2 min of boiling, whereas DBCAA was removed after boiling chlorinated water for 1 min. Trihalomethane concentrations were reduced in both chloraminated (74-98%) and chlorinated (64-98%) water upon boiling. Boiling chloraminated water for 1 min reduced chloroform concentration by 75%. Chloroform was reduced by only 34% in chlorinated water after a 1 min boil, which indicates that simultaneous formation and volatilization of chloroform was occurring. Most of the remaining DBPs (e.g. haloketones, chloral hydrate, haloacetonitriles) were removed by at least 90% after 1 min of boiling in both samples. These data suggest that other mechanisms (e.g., hydrolysis) may have been responsible for removal of the non-volatile DBPs and further highlight the importance of examining individual species when estimating thermal effects on DBP concentrations.  相似文献   

7.
The aim of this paper was to assess the extent of biodegradable dissolved organic carbon formation upon disinfection of water with chlorine dioxide. Wide diversity of natural waters has been subjected to reactions with various amounts of ClO2. For comparison examined waters have also been treated with ozone and chlorine. The application of chlorine dioxide and ozone significantly changed the molecular weight distribution of aquatic organic matter. As a result significant amounts of biodegradable carboxylic acids and aldehydes were generated. The formic, acetic, oxalic and ketomalonic acids as well as formaldehyde, acetaldehyde, glyoxal, methylglyoxal were identified. The productivity of aldehydes calculated for all examined waters and disinfectants amounted 12.7-47.7 μg mg−1 DOC in the case of ozonation, 1.3-8.1 μg mg−1 DOC after chlorination and 1.7-9.4 μg mg−1 DOC for ClO2 treatment. The highest total concentration of carboxylic acids was determined after the ozonation processes. In this case the organic acids' formation potential was in the range 10.8-62.8 μg mg−1 DOC. Relatively high formation potential (5.3-17.9 μg mg−1 DOC) was determined after the oxidation with ClO2 as well. In the case of chlorination, the productivity of organic acids was low and did not exceed 3.4 μg mg−1 DOC. The relatively high correlation between BDOC formation and carboxylic acids' formation potential was observed. Thus, carboxylic acids' formation potential may be used as a measure of water potential to form BDOC.  相似文献   

8.
The formation of disinfection by-products (DBPs) is a public health concern. An important way to evaluate the presence of DBPs is in terms of the total organic halogen (TOX), which can be further specified into total organic chlorine (TOCl), bromine (TOBr), and iodine (TOI). The formation and distribution of halogen-specific TOX during chlorination and chloramination of natural organic matter (NOM) isolates in the presence of bromide and iodide ions were studied. As expected, chloramination produced significantly less TOX than chlorination. TOCl was the dominant species formed in both chlorination and chloramination. TOI was always produced in chloramination, but not in chlorination when high chlorine dose was used, due to the limited presence of HOI in chlorination as a result of the oxidation of iodide to iodate in the presence of excess chlorine. The formation of TOI during chloramination increased as the initial iodide ion concentration increased, with a maximum of ∼60% of the initial iodide ion becoming incorporated into NOM. Iodine incorporation in NOM was consistently higher than bromine incorporation, demonstrating that the competitive reactions between bromine and iodine species in chloramination favoured the formation of HOI and thus TOI, rather than TOBr. Correlations between the aromatic character of the NOM isolates (SUVA254 and % aromatic C) and the concentrations of overall TOX and halogen-specific TOX in chloramination were observed. This indicates that the aromatic moieties in NOM, as indicated by SUVA254 and % aromatic C, play an important role in the formation of overall TOX and halogen-specific TOX in chloramination. THMs comprised only a fraction of TOX, up to 7% in chloramination and up to 47% in chlorination. Although chloramine produces less TOX than chlorine, it formed proportionally more non-THM DBPs than chlorine. These non-THM DBPs are mostly unknown, corresponding to unknown health risks. Considering the higher potential for formation of iodinated DBPs and unknown DBPs associated with the use of chloramine, water utilities need to carefully balance the risks and benefits of using chloramine as an alternative disinfectant to chlorine in order to satisfy guideline values for THMs.  相似文献   

9.
Artificial neural network (ANN) models were developed to predict disinfection by-product (DBP) formation during municipal drinking water treatment using the Information Collection Rule Treatment Studies database complied by the United States Environmental Protection Agency. The formation of trihalomethanes (THMs), haloacetic acids (HAAs), and total organic halide (TOX) upon chlorination of untreated water, and after conventional treatment, granular activated carbon treatment, and nanofiltration were quantified using ANNs. Highly accurate predictions of DBP concentrations were possible using physically meaningful water quality parameters as ANN inputs including dissolved organic carbon (DOC) concentration, ultraviolet absorbance at 254 nm and one cm path length (UV254), bromide ion concentration (Br), chlorine dose, chlorination pH, contact time, and reaction temperature. This highlights the ability of ANNs to closely capture the highly complex and non-linear relationships underlying DBP formation. Accurate simulations suggest the potential use of ANNs for process control and optimization, comparison of treatment alternatives for DBP control prior to piloting, and even to reduce the number of experiments to evaluate water quality variations when operating conditions are changed. Changes in THM and HAA speciation and bromine substitution patterns following treatment are also discussed.  相似文献   

10.
A sampling program has been undertaken to investigate the variations of disinfection by-products (DBPs) formation and nature and fate of natural organic matter (NOM) through water treatment plants in Istanbul. Specific focus has been given to the effect seasonal changes on the formation of DBPs and organic precursors levels. Water samples were collected from the three reservoirs inlet and within three major water treatment plants of Istanbul, Turkey. Changes in the dissolved organic carbon (DOC), ultraviolet absorbance at 254 nm (UV(254)), specific ultraviolet absorbance (SUVA), trihalomethane formation potential (THMFP), and haloacetic acids formation potential (HAAFP) were measured for both the treated and raw water samples. The variations of THM and HAA concentrations within treatment processes were monitored and also successfully assessed. The reactivity of the organic matter changed throughout the year with the lowest reactivity (THMFP and HAAFP) in winter, increasing in spring and reaching a maximum in fall season. This corresponded to the water being easier to treat in fall and an increase in the proportion of hydrophobic content. Understanding the seasonal changes in organic matter character and their reactivity with treatment chemicals should lead to a better optimization of the treatment processes and a more consistent water quality.  相似文献   

11.
Rodriguez MJ  Serodes J  Roy D 《Water research》2007,41(18):4222-4232
Most research on the occurrence of chlorinated disinfection by-products (DBPs) in drinking water has focused on trihalomethane (THM) formation and evolution, in particular within distribution systems. In this research, we investigated the variability of the occurrence of haloacetic acids (HAAs) during the treatment process in two facilities where surface water is pre-chlorinated before being treated by conventional physico-chemical processes. The investigation focused on both seasonal and point-to-point fluctuations of HAAs. In both facilities, samples were collected weekly during 1 complete year at four points in order to generate robust data on HAAs and on complementary parameters. The results showed that the initial formation of HAAs was the highest and the most variable in the plant where levels of DBP precursor indicators and the pre-chlorination dose were both higher and more variable. Subsequent formation of HAAs from the pre-chlorination point until the settled water occurred due to remaining levels of residual chlorine and DBP precursors. However, HAA levels and in particular dichloroacetic acid (DCAA) (the preponderant HAA species in the waters under study) decreased dramatically during filtration, very probably because of biodegradation within the filter. The effect of filtration on DCAA fate was season-dependant, with the highest degradation in warm water periods and practically no variation during winter. Statistical modeling was applied to empirically identify the operational factors responsible for HAA formation and fate. Model performance to identify HAA variability in waters following pre-chlorination was much better than for water following filtration, which is due to the lack of information on mechanisms and conditions favoring DCAA degradation.  相似文献   

12.
Geme G  Brown MA  Simone P  Emmert GL 《Water research》2005,39(16):3827-3836
A capillary membrane sampling-flow injection analysis method is presented for selectively measuring the concentrations of total trihalomethanes (THMs) and total haloacetic acids (HAAs) in drinking water. The method is based on the reaction between nicotinamide and THM or HAA species to yield a fluorescent product. Two configurations are presented, one selective for total THMs and another selective for total HAAs. The construction of a capillary membrane sampler is described, and the results of method detection limit, accuracy and precision studies are reported for each method. Interference, selectivity and linearity studies are reported as well as the effect of temperature and ionic strength changes. Drinking water samples were analyzed by each proposed method and the results were compared to USEPA methods 502.2 and 552.3.  相似文献   

13.
A comparison of the role of two blue-green algae in THM and HAA formation   总被引:8,自引:0,他引:8  
The contribution of two blue-green algae species, Anabaena flos-aquae and Microcystis aeruginosa, to the formation of trihalomethanes (THMs) and haloacetic acids (HAAs) was investigated. The experiments examined the formation potential of these disinfection by-products (DBPs) from both algae cells and extracellular organic matter (EOM) during four algal growth phases. Algal cells and EOM of Anabaena and Microcystis exhibited a high potential for DBP formation. Yields of total THMs (TTHM) and total HAAs (THAA) were closely related to the growth phase. Reactivity of EOM from Anabaena was slightly higher than corresponding cells, while the opposite result was found for Microcystis. Specific DBP yields (yield/unit C) of Anabaena were in the range of 2-11 μmol/mmol C for TTHM and 2-17 μmol/mmol C for THAA, while those of Microcystis were slightly higher. With regard to the distributions of individual THM and HAA compounds, differences were observed between the algae species and also between cells and EOM. The presence of bromide shifted the dominant compounds from HAAs to THMs.  相似文献   

14.
Huseyin Selcuk 《Water research》2010,44(13):3966-6140
In this study, disinfection and formation of disinfection by-products (DBPs) were studied in a photoelectrocatalytic (PEC) treatment system. Disinfection performance of titanium dioxide (TiO2) in the PEC system was determined through Escherichia coli (E. coli) inactivation. Humic acid (HA) was used as a model organic compound and its removal was monitored by total organic carbon (TOC) measurements using 410 nm (color) and 254 nm (UV254) wavelengths. Trihalomethanes (THMs) were measured for the evaluation of DBPs formation during PEC treatment of chloride and HA mixture. It was found that unlike photocatalytic treatment, THMs might form in the PEC system. To investigate the effects of anions on the PEC treatment, chloride (Cl), sulfate (SO42−), phosphoric acid (H2PO4)/hydrogen phosphate (HPO42−) and bicarbonate (HCO3) ions were added separately to the HA and bacterial suspensions. Presence of H2PO4/HPO42− and HCO3 ions resulted in inhibitory effects on both HA degradation and E. coli inactivation, which were also examined in the photoanode. It was observed that the presence of HA had a strong inhibitory effect on the disinfection of E. coli.  相似文献   

15.
Chlorine is typically used within drinking water distribution systems to maintain a disinfectant residual and minimize biological regrowth. Typical distribution system models describe the loss of disinfectant due to reactions within the water matrix as first order with respect to chlorine concentration, with the reactants in excess. Recent work, however, has investigated relatively simple dynamic models that include a second, hypothetical reactive species. This work extends these latter models to account for discontinuities associated with rechlorination events, such as those caused by booster chlorination and by mixing at distribution system junction nodes. Mathematical arguments show that the reactive species model will always represent chlorine decay better than, or as well as, a first-order model, under single dose or rechlorination conditions; this result is confirmed by experiments on five different natural waters, and is further shown that the reactive species model can be significantly better under some rechlorination conditions. Trihalomethane (THM) formation was also monitored, and results show that a linear relationship between total THM (TTHM) formation and chlorine demand is appropriate under both single dose and rechlorination conditions. This linear relationship was estimated using the modeled chlorine demand from a calibrated reactive species model, and using the measured chlorine demand, both of which adequately represented the TTHM formation.  相似文献   

16.
This study demonstrates that levels of trihalomethanes (THMs) increase considerably when cold water stagnates in residential pipes and, more significantly, when water remains in the hot water tank. Levels of haloacetic acids (HAAs) increase as well in both cases, but less significantly in comparison to THMs. The study also demonstrates that in both the plumbing system and residential hot water tank, chlorinated and brominated DBP species do not behave in the same manner. Finally, the study shows that sustained use of water in households helps to maintain THM and HAA levels close to those found in water of the distribution system. The results are useful to identify methods of indoor water use that minimize population exposure to DBPs and improve DBP exposure assessment for epidemiological studies.  相似文献   

17.
Wang W  Ren S  Zhang H  Yu J  An W  Hu J  Yang M 《Water research》2011,45(16):4930-4938
Due to their high carcinogenicity, the control of nitrosamines, a group of disinfection by-products (DBPs), is an important issue for drinking water supplies. In this study, a method using ultra-performance liquid chromatography-electrospray ionization tandem mass spectrometry was improved for simultaneously analyzing nine nitrosamines in source water and finished water samples of twelve drinking water treatment plants (DWTPs) in China. The method detection limits of the nine target analytes were 0.2-0.9 ng/L for the source water samples and 0.1-0.7 ng/L for the finished water samples. Of the nine nitrosamines, six (N-nitrosodimethylamine (NDMA), nitrosodiethylamine (NDEA), N-nitrosomorpholine (NMor), N-nitrosodi-n-butylamine (NDBA), N-nitrosomethylethylamine (NMEA), and N-nitrosodiphenylamine (NDPhA)) were detected. The total nitrosamine concentrations in source water and finished water samples were no detection-42.4 ng/L and no detection-26.3 ng/L, respectively, and NDMA (no detection-13.9 ng/L and no detection-20.5 ng/L, respectively) and NDEA (no detection-16.3 ng/L and no detection-14.0 ng/L, respectively) were the most abundant. Meanwhile, the occurrence of nine secondary amines corresponding to the nine nitrosamines was also investigated. All of them except for di-n-propylamine were detected in some source water and finished water samples, and dimethylamine (no detection-3.9 μg/L and no detection-4.0 μg/L, respectively) and diethylamine (no detection-2.4 μg/L and no detection-1.8 μg/L, respectively) were the most abundant ones. Controlled experiments involving chloramination of four secondary amines confirmed that dimethylamine, diethylamine, morpholine and di-n-butylamine in water can form the corresponding nitrosamines, with diethylamine and morpholine showing significantly higher yields than dimethylamine which has already been identified as a precursor of NDMA. This study proved that diethylamine, morpholine and di-n-butylamine detected in raw water would be one of the important the precursors of NDEA, NMOR and NDBA, respectively, in drinking water.  相似文献   

18.
Kanan A  Karanfil T 《Water research》2011,45(2):926-932
The contribution and role of different precursors in the formation of three class of disinfection by-products (DBPs) [trihalomethanes (THMs), haloacetic acids (HAAs), and halonitromethanes (HNMs)] in swimming pool waters were examined using filling waters obtained from five drinking water treatment plant (WTP) effluents and three body fluid analogs (BFAs). BFAs exerted higher chlorine demands as compared to natural organic matter (NOM) in filling waters. BFAs exhibited higher HAA formation potentials than THM formation potentials, while the opposite was observed for the filling water NOM. There was no appreciable difference in the HNM formation potentials of BFAs and filling water NOM. Different components in the BFAs tested exhibited different degree and type of DBP formation. Citric acid had significantly higher THM and HAA yields than other BFA components. The effect of temperature was greater on THM formation, whereas the effect of contact time had more impact on HAA formation. Experiments with filling waters collected from WTP effluents at three different times showed more variability in HAA than THM formation at the WTPs studied.  相似文献   

19.
Sirivedhin T  Gray KA 《Water research》2005,39(6):1025-1036
In this study, the chemical reactivity with chlorine as measured by disinfection by-product formation potential (DBPFP) is compared among samples of a wastewater effluent and surface waters. Water samples that had higher anthropogenic impacts were found to have higher overall DBPFP due primarily to higher dissolve organic carbon (DOC) concentrations. Effluent-derived organic matter (EfOM), however, was found to be less reactive with chlorine on a per DOC concentration basis. Yet, EfOM had higher proportions of brominated DBP, which may be associated with greater health risks. In this research, pyrolysis-GC/MS was used to establish relationship between structural features of DOC and DBPFP. We show that there is a critical set of pyrolysis fragments that separates the waters based on the degree of anthropogenic influence. Even though no single chemical marker was found to be indicative of the formation potentials of different classes of DBP, combinations of chemical fragments were found to be associated with the formation potentials of total trihalomethane (THM), brominated THM, total haloacetic acid (HAA), and brominated HAA for this set of samples. In contrast to previous work, the phenolic signature of these samples was negatively correlated to DBPFP, whereas strong relationships were found between DBPFP and the organic nitrogen and halogenated signatures.  相似文献   

20.
In this study, different tap water handling strategies were investigated to evaluate the effects on two principal chlorinated DBPs, trihalomethanes (THMs) and haloacetic acids (HAAs). Tap water samples collected in the Quebec City (Canada) distribution system on a spatio-temporal basis were subjected to diverse indoor handling scenarios: storing water in the refrigerator, boiling water followed by storage and, finally, filtering water with a point-of-use commercial pitcher also followed by storage. In the first two cases, the use of covered and uncovered pitchers was investigated separately, while in the last case, both the use of new and used filters was compared. In all cases, maximum storage time was 48h. Results demonstrated that in some cases, water handling scenarios have considerable effect, and in other cases, little or no effect. Removal of THM concentrations by simple storage was high (on average 30%) and very high by boiling and filtering with subsequent storage in the refrigerator (on average, 87% and 92%, respectively). In scenarios where water was stored in uncovered pitchers (with or without previous boiling and filtering), the THM decrease was higher for increased storage times. However, storage did not have any effect on HAAs, whereas boiling decreased levels of trichloroacetic acid (TCAA) (on average 42%) and increased levels of dichloroacetic acid (DCAA) (on average 35%), resulting in unchanged average levels of total HAAs. The use of the filtration pitcher decreased HAA levels dramatically (on average 66%). Percentages of change in chlorinated DBPs in the different scenarios varied according to initial concentrations in tap water (baseline water), that is, according to the spatio-temporal variations of these substances in the distribution system. On the basis of these results, the paper discusses implications regarding public health protection and exposure assessment for epidemiological studies.  相似文献   

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