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1.
A new sensitive analytical procedure has been developed for the determination of residues of endosulfan in human blood samples. The method involves the extraction of residues of endosulfan from blood samples by the addition of 60% sulfuric acid at 10 degrees C, liquid/liquid partitioning by using hexane and acetone mixture (9:1) and quantification by using GC-ECD. Residues of endosulfan in blood samples were quantified as the sum of alpha-endosulfan, beta-endosulfan, endosulfan sulfate and endosulfandiol. The influence of temperature during the extraction has been studied. Recovery experiments were conducted over the concentration range 1.0-50 ng ml(-1) and the relative standard deviation calculated. The method was found to be sufficiently sensitive to quantify the residue of total endosulfan up to the 1.0 ng ml(-1) level. The recovery was 92% with a calculated relative standard deviation of 1.96%. Conversion of endosulfan to endosulfandiol is found to be less than 0.5% under the defined conditions. The method was applied to the analysis of residue contents of endosulfan and its metabolites in blood samples collected from the exposed population. The data obtained has been confirmed by GC-MS-EI in selective ion monitoring (SIM) mode.  相似文献   

2.
This paper assesses the uptake of persistent organic pollutants (POP's) into plants. In particular, uptake of alpha-endosulfan, beta-endosulfan and endosulfan sulfate from lettuce. The lettuce plants were grown on compost that had previously been contaminated at 10 and 50 microg g(-1) per POP. The soil was slurry spiked by adding the appropriate amount of POP in acetone in an approximate ratio of 1 ratio 2, w/v soil ratio solvent. The solvent was left to evaporate at ambient temperature for 24 hours. Lettuce plants were grown under artificial daylight for 12 hours a day. The influence of soil ageing on the recovery of POP's from spiked soil samples was also assessed. The average recovery of endosulfan compounds from slurry spiked soil (10, 20 and 40 microg g(-1)) was consistent (92.9 +/- 4.4% for n= 9). However, ageing of endosulfan compounds on the slurry spiked soil resulted in lower recoveries (average losses were 12.5% after 14 days ageing of slurry spiked soil). The uptake of POP's was assessed by measuring the amount of endosulfan compounds in roots and leaves from lettuce plants after 10, 20 and 33 days. In addition, control plants grown in uncontaminated soil were monitored and analysed. It was found that endosulfan compounds were present in the roots of all lettuce plants irrespective of soil spike level or age of plant. In the 33 day lettuce plants where the soil was spiked at the highest level (50 microg g(-1)) endosulfan compounds were determined in the leaves. The root to leaf ratio was found to be 3.1 for alpha-endosulfan, 46.0 for beta-endosulfan, and 24.3 for endosulfan sulfate. Spiked lettuce samples were subjected to in vitro gastrointestinal extraction to assess the bioavailability of endosulfan compounds. No detectable endosulfan compounds were determined in the gastric extracts while small quantities (range 0.06-0.12 microg g(-1)) were found in the intestinal extraction. All samples (soil and lettuce) were extracted using pressurised fluid extraction and analysed using gas chromatography with mass selective detection.  相似文献   

3.
Multiple residues of organochlorine insecticides were monitored in the agricultural fields near Farrukhabad in the vicinity of the River Ganga in northern India for one year (1991–1992). Almost all soil samples were found to be contaminated with residues of hexachlorocylohexane (HCH) and dichlorodiphenyl-trichloroethane (DDT). Residues of aldrin and endosulfan were also detected in a large number of samples. Heptachlor residues were scarcely detected. Alpha-HCH, pp-DDT and alpha-endosulfan were found to dominate over the other isomers/metabolites of HCH, DDT and endosulfan, respectively. The average concentration of dieldrin was more than that of aldrin. The concentrations of residues progressively increased up to a depth of 1 m.  相似文献   

4.
Residues of endosulfan insecticide (-and -isomers, and endosulfan sulphate) were determined in the livers of catfish from a cotton growing area during the summer and winter of 1988. The concentration of total endosulfan residues found in the fish was up to 0.31 mg kg-1 wet wt. It decreased in winter with a maximum 0.02 mg kg-1 wet wt. The difference in endosulfan residues between seasons was statistically significant (ANOVA,p<0.01).  相似文献   

5.
One of the most common pesticides in the developing world, endosulfan, can be detected in ppm levels using gold nanoparticles. Endosulfan adsorbs on the nanoparticle surface and upon interaction for a long time, the nanoparticles precipitate from the solution. Interaction with silver is weak, yet adsorption occurs leading to removal of endosulfan from the solution. A multilayer assembly of gold nanoparticles prepared on a glass substrate shows excellent spectrophotometric response suggesting potential applications.  相似文献   

6.
Multiple residues of organochlorine insecticides were monitored in Ganga river water in the district of Farrukhabad in northern Indian for one year (1991–1992). Almost all the samples were found to be contaminated with residues of HCH and DDT. Residues of aldrin, endosulfan and heptachlor were also detected in a larger number of samples. Alpha-HCH, pp-DDT and alpha-endosulfan were found to dominate over the other isomers of HCH, DDT and endosulfan, respectively. Enhanced percentage of beta-HCH suggests accumulation of this isomer in the aquatic environment. The average concentration of aldrin was more than that of dieldrin. Aldrin residues often exceeded the WHO guideline value for drinking water and the concentration of heptachlor occasionally exceeded the specified limits.  相似文献   

7.
In the present study we quantified the residues of organophosphorus (e.g. ethion and chlorpyrifos), organochlorine (e.g. heptachlor, dicofol, alpha-endosulfan, beta-endosulfan, endosulfan sulfate) and synthetic pyrethroid (e.g. cypermethrin and deltamethrin) pesticides in made tea, fresh tea leaves, soils and water bodies from selected tea gardens in the Dooars and Hill regions of West Bengal, India during April and November, 2006. The organophosphorus (OP) pesticide residues were detected in 100% substrate samples of made tea, fresh tea leaves and soil in the Dooars region. In the Hill region, 20% to 40% of the substrate samples contained residues of organophosphorus (OP) pesticides. The organochlorine (OC) pesticide residues were detected in 33% to 100% of the substrate samples, excluding the water bodies in the Dooars region and 0% to 40% in the Hill region. The estimated mean totals of studied pesticides were higher in fresh tea leaves than in made tea and soils. The synthetic pyrethroid (SP) pesticide residues could not be detected in the soils of both the regions and in the water bodies of the Dooars. Sixteen percent and 20% of the made tea samples exceeded the MRL level of chlorpyrifos in Dooars and Hill regions respectively. The residues of heptachlor exceeded the MRL in 33% (April) and 100% (November) in the Dooars and 40% (April) and 20% (November) in the Hill region. Based on the study it was revealed that the residues of banned items like heptachlor and chlorpyrifos in made tea may pose health hazards to the consumers.  相似文献   

8.
Endosulfan is one of the few organochlorine insecticides still in use in China for protecting crops from a variety of insects. Endosulfan is toxic in fishes and rodents in the in vivo assays, but its genotoxicity in mammalian cells has not been well tested. In this work, a genotoxic testing system has been developed based on the induction of a HepG2/GADD153-GFP reporter gene expression in response to the DNA-damaging agents. Methyl methanesulfonate, a known carcinogenic and genotoxic agent, was used to test the effects of damage dose and post-treatment incubation time on GADD153-GFP expression. Subsequently, the system was applied to the genotoxicity evaluation of endosulfan. Endosulfan was able to cause the increase of GADD153-GFP expression at a sublethal dose (0.02?C20 mg/L). In particular, it induced a maximum green fluorescent protein expression at the tested concentration of 0.2 mg/L, with 4.07-fold inflorescence relative to untreated cells. The results suggest that endosulfan has the potential genotoxicity for HepG2 cell line by inducing DNA damage. The study also confirms that the induced GADD153-GFP expression system is an appropriate and sensitive method for the assessment of genotoxicity from a broad range of pesticides with the DNA-damaging potential.  相似文献   

9.
Analysis of endosulfan, chlorpyrifos, and their nonpolar metabolites in extracts from environmental aqueous and soil samples was performed using a gas chromatography-tandem mass spectrometry (GC–MS/MS) technique. Full-scan GC–MS analysis showed poor sensitivity for some of the metabolites (endodiol and endosulfan ether). A multisegment MS/MS method was developed and MS/MS parameter isolation time, excitation time, excitation voltage, and maximum excitation energy were optimized for chosen precursor ions to enhance selectivity and sensitivity of the analysis. The use of MS/MS with optimized parameters quantified analytes with significantly higher accuracy, and detection limits were lowered to ~1/6th compared with the full-scan method. Co-eluting compounds, chlorpyrifos and chlorpyrifos oxon, were also analyzed successfully in the MS/MS mode by choosing exclusive precursor ions. Analysis of soil and water phase samples from contaminated soil slurry bioreactors showed that the MS/MS method could provide more reliable estimates of these pesticide and metabolites (especially those present in low concentrations) by annulling interferences from soil organic matter.  相似文献   

10.
Endosulfan, a persistent organic pollutant newly listed under the Stockholm Convention, is currently widely produced and used as a pesticide in China. Concentrations of endosulfans (including α-, β-isomers, and their metabolite endosulfan sulfate) were determined in surface soil collected from Huai’an city, where the largest endosulfan producer is located. The concentrations of Σendosulfan (sum of α-endosulfan, β-endosulfan, and endosulfan sulfate) at all sites ranged from 0.28 to 44.81?ng/g dry weight (dw), following a lognormal distribution. The geometric mean was 1.09?ng/g dw, and the geometric standard deviation was 3.02. The β-endosulfan levels were consistently greater than those of α-isomer. The concentration ratios of α-endosulfan to β-endosulfan ranged from 0.03 to 0.70, which were much lower than the commercial endosulfan mixture. This is because that α-endosulfan is more volatile and degrades faster than β-endosulfan in soil. The contour map of Σendosulfan levels in soil indicates that the factory was the point pollution source with the highest endosulfan level in its surrounding area, especially the southern area. However, the non-point agricultural sources are more important. Based on Monte Carlo simulation, the Σendosulfan inventory in soil in Huai’an is estimated to be 0.8–3.0 tons. In order to understand the potential ecological risk of endosulfan, the Monte Carlo-based hazard quotient distribution was estimated and showed that Σendosulfan posed a potentially high risk to soil organisms. To our knowledge, this study is the first that reports soil pollution and risk of endosulfan around the manufacturer in China. This study will help China’s implementation of Stockholm Convention for the reduction and elimination of endosulfan in future.  相似文献   

11.
An assessment of levels of endosulfan and endosulfan sulphate in rats collected from a plot sprayed with endosulfan was carried out for a period of four months. The analysis was carried out in the livers, muscles and fatty tissues of the rats using Gas Chromatography. Samples were ground with sodium sulphate and aluminium oxide and the analyte soxhlet extracted with hexane. The extract was then cleaned by florisil column chromatography. Levels of endosulfan in rats were found to range in livers from 0.356 to 5.807 ppb, in muscles from 0.089 to 5.167 ppb and in fatty tissues from 0.083 to 4.785 ppb. Levels of endosulfan sulphate correlated well with those of endosulfan and ranged in livers from 0.00 to 3.96 ppb, in muscles from 0.00 to 3.37 ppb and in fatty tissue from 0.00 to 2.93 ppb. In the control rats samples, collected from an unsprayed area in the city of Harare (University of Zimbabwe), no endosulfan could be detected.  相似文献   

12.
A procedure to assess the bioavailability of persistent organic pollutants (POPs) from soil samples has been developed. The procedure is based on the use of simulated in vitro gastrointestinal extraction to remove POPs from soil matrices. The level of recovery, using this approach, is assessed following liquid-liquid extraction (LLE) and analysis by gas chromatography-mass selective detection (GC-MSD). The remaining soil residue is then extracted using pressurised fluid extraction (PFE) followed by GC-MSD analysis to assess the residual fraction. The residual fraction is monitored to determine the unavailable fraction i.e. not available for absorption in the gastrointestinal tract of humans. The procedure was applied to four soil samples i.e. an aged, spiked soil and three certified reference materials (CRMs) contaminated with POPs. Recoveries of pesticides (lindane, endosulfan I, endrin, DDE, DDD and endosulfan II), phenols (cresol, TCP and PCP), and base neutral compounds (hexachloroethane, acenaphthene, dibenzofuran, fluorene and hexachlorobenzene) from aged, spiked soil following extraction with gastric fluid ranged from 0.8 to 8.3% while following intestinal extraction ranged from 5.5 to 13.5%, irrespective of POP. Recoveries of pesticides (lindane, endosulfan I, endrin, DDE, DDD and endosulfan II) from CRM 805-050 following extraction with gastric fluid were below the limit of detection while following intestinal extraction ranged from 5.3 to 12.8%. Recoveries of phenols (cresol, TCP and PCP) from CRM 401-225 following extraction with gastric fluid ranged from 1.6 to 2.0% while following intestinal extraction ranged from 4.1 to 5.4%. Recoveries of base neutral acid analytes (hexachloroethane, acenaphthene, dibenzofuran, fluorene and hexachlorobenzene) from CRM 107-100 following extraction with gastric fluid ranged from 1.4 to 4.0% while following intestinal extraction ranged from 6.6 to 12.7%. It has been found that the majority of POPs present i.e. >75%, would be excreted if consumed and not be absorbed in the gastrointestinal tract of humans.  相似文献   

13.
Rapid increase in industrialization and agricultural activities to meet the population need has led to environmental pollution. The major revolution in agricultural production is mainly due to increased use of pesticides and fertilizers. Soil act as a major sink for majority of pesticides applied on agricultural crops. Among the organochlorines, endosulfan is the most commonly used pesticide, hence this study concentrates on the persistence and distribution behaviour of endosulfan under field conditions. The result showed that the alpha endosulfan concentrations were very minimum (0.98 mg/kg of soil) in all the four fields under study (Nazarath, Othikadu, Ekkadu and Ekkadukandigai of Thiruvallur district, Tamil Nadu). Where as beta endosulfan concentration at the time of application was 6.39 mg/kg and declined to 0.8 mg/kg on soil at 150th day. The endosulfan sulfate concentration was 11.8 mg/kg in soil at 15th day and then concentration declined to 2.2 mg/kg at 150th day. Field run-off samples showed maximum residue levels (0.024 mg/l) at the early irrigation period. While plant foliar parts showed maximum concentrations of α-endosulfan (43.4 mg/kg), β-endosulfan (40.6 mg/kg) and endosulfan sulfate (20.1 mg/kg). At harvest stage, rice grain and husk also had lower concentrations of endosulfan sulfate (2.2 and 0.09 mg/kg), respectively.  相似文献   

14.
The residual levels of organochlorine pesticides (OCPs) in the dust fall around Lake Chaohu were measured using gas chromatography mass spectrometry from April 2010 to March 2011. The fluxes, components, temporal–spatial variations, and sources of OCPs were also analyzed. Twenty-one types of OCPs were detected in the dust fall samples around Lake Chaohu, with a total concentration of 51.54?±?36.31 ng/g and a total flux of 10.01?±?13.69 ng/(m2 day). Aldrin (35.3 %), endosulfan (39.1 %), dichlorodiphenyltrichloroethanes (DDTs) (49.8 %), and isodrin (37.1 %) were the major OCPs in the spring, summer, autumn, and winter, respectively. Both the residual level and the flux were higher in the spring than in other seasons and higher at the outer lake sampling sites than inner lake sampling site. The potential source of the hexachlorcyclohexanes in the dust fall may be recent lindane usage. The DDTs mainly came from historical dicofol usage, and a significant input of DDT was found during April and June. The presence of endosulfan may be due to the present use of technical endosulfan. The aldrin in the dust might be due to its occasional usage, and isodrin may be a result of long-distance transport from other countries.  相似文献   

15.
This paper documents levels of organochlorine pesticides (OCs) in coastal surface sediments from selected reference sites on the northern Atlantic Spanish coast. One hundred eight samples covering three estuaries in the Cantabrian Coast were sampled in 2006 and analyzed in the finer fraction (<63 ??m) for 19 OCs by gas chromatography with electron capture detector after confirmation by mass spectrometry. Detected organochlorine pesticides were endosulfan ??, endosulfan ??, endosulfan sulfate, hexachlorobenzene (HCB), aldrin, dieldrin, methoxychlor, 1,1-dichloro-2,2-bis(4-chlorophenyl)ethylene (4,4??-DDE) and 1,1-dichloro-2,2-bis(4-chlorophenyl)ethane (4,4??-DDD). Total OCs concentrations ranged from 1.8 ng g???1 dry weight (dw) to 3.9 ng g???1 dw, showing a uniform distribution along the studied area, and being consistent with recorded levels in the literature for coastal sediments in other reference sites with low levels of pollution by OCs along the Atlantic Ocean. Endosulfan, 4,4??-DDD, HCB, aldrin, and dieldrin seemed to be ubiquitous as the legacy of past uses and deposition. OCs concentrations were significantly correlated to organic matter content and particle size distribution. No adverse biological effects derived from these pollutants are expected to take place as it can be concluded from the comparison with the existent marine sediment quality guidelines.  相似文献   

16.
Green mussel (Perna viridis) and water samples were collected from Ennore creek, Chennai by seasonal sampling and analyzed for organochlorine pesticide residues (OCPs) like dichloro-diphenyl-trichloroethane (DDT) and its metabolites, isomers of hexachlorocyclohexane (HCH) and endosulfan. These residues were analyzed by using gas chromatograph (GC) with μECD. In the present study, mussel samples showed very low concentrations of OCPs in the statistical order of DDT (5.83 ng g???1 wet tissue) > endosulfan (2.84 ng g???1 wet tissue) > HCH (2.34 ng g???1 wet tissue). Concentrations of OCPs in water samples were in the statistical order of endosulfan (29.21 ng L???1)?> HCH (17.14 ng L???1)?> DDT (14.63 ng L???1). To our knowledge, this is the first report on the seasonal variation of OCPs and especially the quantification of endosulfan in Ennore Creek. The present study recommends that continuous monitoring in Ennore creek is necessary to assess possible impact on human health.  相似文献   

17.
The extent of contamination by endosulfans in soil samples collected from the Point Mugu watershed near Oxnard, California was determined using capillary gas chromatography/mass selective detection (GC/MSD). The study was designed to detect three organochlorinated pesticides: endosulfan , endosulfan and endosulfan sulfate. Thirteen sets of two soil samples each were taken from various sites in the region. Our results show that the endosulfan levels in these soils range from trace amounts to nearly 30 ppm, with endosulfan being the most abundant and endosulfan sulfate the least. Two sites of the study, Hueneme and Revolon and Farm and Revolon, showed high amounts of endosulfans and , with concentrations between 20 and 30 ppm. The majority of the other sites studied in this research produced concentrations of less than 10 ppm for each of the three endosulfans monitored. At five areas in particular, Pleasant Valley and Creek, Laguna and Creek, Etting and Creek, Road and Creek and Hueneme and Creek, less than 2 ppm or only trace amounts of endosulfans , and sulfate were detected.  相似文献   

18.
The integrated pest management (IPM) modules of pesticide schedule on Basmati rice were validated at field experiments conducted in Northern India for consecutive 3 years (2005–2008). The pesticide residues were found below the detectable limit (<0.01–0.001 mg/kg) in soil and irrigation water samples of Kaithal region. In Dehra Dun region of Uttrakhand, the residues of carbendazim in rice grains and soil were detected below <0.01 mg/kg level. In second year experiments (2006–2007), only four non-IPM soil samples indicated the presence of chlorpyrifos and endosulfan in the range of ND <0.001 to 0.07 mg/kg, out of 45 samples analyzed. Carbendazim applied as seed treatment at Dehradun and Kaithal field trials was found below detectable limit in both IPM and non-IPM rice grains (<0.01 mg/kg) and irrigation water (0.01 μl/ml). Chlorpyrifos was detected in five water samples from Kaithal and one from Pant Nagar in the range of 0.003–0.006 μl/L, α- and β-isomer of endosulfan in the range of 0.005–0.03, and 0.005–0.02 μl/ml, respectively, in one sample from Pant Nagar and two from Kaithal, out of a total of 22 samples. In the region of Uttrakhand and Uttar Pradesh during 2007–2008, four non-IPM samples of soil indicated trace levels of endosulfan, out of 16 samples analyzed. The residues were detected below detection limit for carbendazim (<0.01 mg/kg) in soil samples of Dehradun IPM fields and for endosulfan and carbendazim (0.001–0.01 μl/L) in water samples each from IPM and non-IPM fields of Uttar Pradesh. The results of 3-year trials of IPM module indicated basmati rice as safe and economical with pesticide residue-free rice grains.  相似文献   

19.
Organochlorine pesticides in the soil of a karst cave in Guilin, China   总被引:1,自引:0,他引:1  
Organochlorine pesticides (OCPs) including HCH, DDT, chlordane, endosulfan, and endosulfan sulfate were analyzed in surface soil of the Dayan Cave to investigate their source and concentration levels in September 2006. Generally, the data showed that outside soil of the cave had much higher concentrations than inside soil for the most detected OCPs in the cave and both inside soil and outside soil showed much lower concentration levels (basically, the levels of OCPs were less than 0.7 ng/g) than those observed in other regions within and outside China other than TC (ranging from 3.22 to 5.00 ng/g) and CC (ranging from 3.89 to 5.08 ng/g) in the soil outside. The ratios of α-/γ-HCH ranged from 0.88 to 1.20 in the soil of the cave, together with the averaged percentages of β-HCH and δ-HCH among the total HCH isomers (accounting for 39.0% and 14.2%, respectively), implied that a historical residue of local technical HCH contamination was likely to be dominant in the soil of the cave. Based on (1) the accordance of TC/CC ratios (ranging from 0.83 to 0.98) between the values observed in the outside soil and the potentially available chlordane products in the markets, and (2) the high concentrations of TC and CC observed in the outside soil, it appeared that the illegal usage of technical chlordane was done in Guilin. The low concentrations of TC (0.02 to 0.56 ng/g) and CC (0.10 to 1.71 ng/g) in the inside soil, together with the significant distinctions of TC/CC ratios between the inside soil (ranging from 0.03 to 0.33) and the outside soil, implied that the chlordane in the inside soil of the cave was a historical residue of local technical chlordane contamination. The similar ratios of DDT isomers (o,?p (')-DDT/p,?p (')-DDT and p,?p (')-DDE+DDD/DDT) between the outside soil and the inside soil of the cave suggested that they may have the similar DDT source. The ratios of p,?p (')-DDE+DDD/DDT (ranging from 3 to 8) indicated that DDT was relatively aged. The values of o,?p (')-DDT/p,?p (')-DDT ratios (ranging from 3 to 7.5 with a mean value of 5.45) were found to be much higher than that of technical DDT, and very similar to that of dicofol products, implied that the primary source of DDT in the soil of the cave was most probably from dicofol-type DDT products. The low concentration levels of endosulfan and the higher levels of metabolite endosulfan sulfate indicated that the residue from historical usage of technical endosulfan was likely to be dominant in the soil of the cave.  相似文献   

20.
The CA Department of Pesticide Regulation (CDPR) and the CA Air Resources Board monitored 40 pesticides, including five degradation products, in Parlier, CA, to determine if its residents were exposed to any of these pesticides and, if so, in what amounts. They included 1,3-dichloropropene, acrolein, arsenic, azinphos-methyl, carbon disulfide, chlorpyrifos and its degradation product, chlorthalonil, copper, cypermethrin, diazinon and its degradation product, dichlorvos, dicofol, dimethoate and its degradation product, diuron, endosulfan and its degradation product, S-ethyl dipropylcarbamothioate (EPTC), formaldehyde, malathion and its degradation product, methyl isothiocyanate (MITC), methyl bromide, metolachlor, molinate, norflurazon, oryzalin, oxyfluorfen, permethrin, phosmet, propanil, propargite, simazine, SSS-tributylphosphorotrithioate, sulfur, thiobencarb, trifluralin, and xylene. Monitoring was conducted 3 days per week for a year. Twenty-three pesticides and degradation products were detected. Acrolein, arsenic, carbon disulfide, chlorpyrifos, copper, formaldehyde, methyl bromide, MITC, and sulfur were detected in more than half the samples. Since no regulatory ambient air standards exist for these pesticides, CDPR developed advisory, health-based non-cancer screening levels (SLs) to assess acute, subchronic, and chronic exposures. For carcinogenic pesticides, CDPR assessed risk using cancer potency values. Amongst non-carcinogenic agricultural use pesticides, only diazinon exceeded its SL. For carcinogens, 1,3-dichloropropene concentrations exceeded its cancer potency value. Based on these findings, CDPR has undertaken a more comprehensive evaluation of 1,3-dichloropropene, diazinon, and the closely related chlorpyrifos that was frequently detected. Four chemicals—acrolein, arsenic, carbon disulfide, and formaldehyde—sometimes used as pesticides were detected, although no pesticidal use was reported in the area during this study. Their presence was most likely due to vehicular or industrial emissions.  相似文献   

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