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1.
Sediments used in this study were selected from 23 stations in the middle and lower reaches of the Yellow River and its tributaries in November 2005. The levels and distribution patterns of selected organochlorine pesticides (OCPs = p,p -DDT, o,p -DDT, p,p -DDE, p,p -DDD, α-, β-, γ-, and δ-HCH) in samples were investigated by analysis of gas chromatography coupled with micro-electronic capture detector. Concentration of OCPs in the sediments from the Yellow River ranged from 0.05 to 5.03 ng g???1 (mean, 1.02 ng g???1) for ∑DDT, 0.09–12.89 ng g???1 (mean, 1.08 ng g???1) for ∑HCH. The concentration distribution of ∑DDT and ∑HCH varied significantly with different sampling station, indicating their different contamination sources. Composition analyses demonstrated that residues of DDTs in sediments came from the previous inputs of organochlorine pesticides, while β-HCH and γ-HCH significantly dominated in the sediments for HCHs.  相似文献   

2.
The concentration of 12 organochlorine pesticides (OCPs) were measured in water, sediment, aquatic plant, and animal (shrimp and fish) of Nansi Lake by gas chromatography equipped with an electron capture detector. The total OCPs concentrations were 65.31–100.31 ng L?1 in water, 2.9–6.91 ng g?1 dry weight (dw) in sediments, 1.29–6.42 ng g?1 dw in aquatic plants and 7.57–17.22 ng g?1 dw in animals. The OCPs composition profiles showed that heptachlor compounds was also the predominant OCPs contaminants in addition to hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) in Nansi Lake. According to the source of HCHs and DDTs in sediment samples, there was no new input and the HCHs pollution mainly came from the use of Lindane in Nansi Lake. Bioaccumulation of OCPs in aquatic biota indicated that DDTs and heptachlor compounds had a strong accumulation, followed by HCHs and drins. The accumulation abilities of fish for OCPs were higher than those of plants and shrimps. The OCPs biota-sediment accumulation factor values of Channa argus was the highest in fish samples, followed by Carassius auratus, and Cyprinus caspio. Risk assessment of sediment showed that heptachlor epoxide had a higher occurrence possibility of adverse ecological effects to benthic species. Based on the calculation of acceptable daily intake and hazard ratio, HCHs in fish and shrimps from Nansi Lake had a lifetime cancer risk of greater than one per million. The risk assessment of water, sediment, and fish indicated the water environment of Nansi Lake is at a safe level at present.  相似文献   

3.
The spatial variability and temporal trend in concentrations of the organochlorine pesticides (OCPs), hexachlorocyclohexane (HCH) and dichlorodiphenyltrichloroethane (DDT), in soils and agricultural corps were investigated on an intensive horticulture area in Hohhot, North-West China, from 2008 to 2011. The most frequently found and abundant pesticides were the metabolites of DDT (p,p′-DDE, p,p′-DDT, o,p′-DDT and p,p′-DDD). Total DDT concentrations ranged from ND (not detectable) to 507.41 ng/g and were higher than the concentration of total HCHs measured for the range of 4.84–281.44 ng/g. There were significantly positive correlations between the ∑DDT and ∑HCH concentrations (r 2>0.74) in soils, but no significant correlation was found between the concentrations of OCPs in soils and clay content while a relatively strong correlation was found between total OCP concentrations and total organic carbon (TOC). β-HCH was the main isomer of HCHs, and was detected in all samples; the maximum proportion of β-HCH compared to ∑HCHs (mean value 54%) was found, suggesting its persistence. The α/γ-HCH ratio was between 0.89 and 5.39, which signified the combined influence of technical HCHs and lindane. Low p,p′-DDE/p,p′-DDT in N1, N3 and N9 were found, reflecting the fresh input of DDTs, while the relatively high o,p′-DDT/p,p′-DDT ratios indicated the agricultural application of dicofol. Ratios of DDT/(DDE+DDD) in soils do not indicate recent inputs of DDT into Hohhot farmland soil environment. Seasonal variations of OCPs featured higher concentrations in autumn and lower concentrations in spring. This was likely associated with their temperature-driven re-volatilization and application of dicofol in late spring.  相似文献   

4.
The levels of hexachlorocyclohexane (HCH) and dichloro-diphenyl-trichloroethane (DDT) in the water, suspended particulate matter (SPM), and sediments from Lake Small Baiyangdian were measured by gas chromatograph with a 63Ni microelectron capture detector. The residual levels of the total HCHs in the water, SPM, and sediments were 1.59?±?2.24 ng L?1, 25.42?±?1.72 ng g?1 dw (dry weight), and 0.86?±?1.44 ng g?1 dw, respectively. DDTs were not detected in the water samples. The concentrations of total DDTs were 158.79?±?1.67 ng g?1 dw in SPM and 0.46?±?1.97 ng g?1 dw in the sediments. Compared to other areas in China and abroad, the levels of residual HCH and DDT were relatively low in the water and sediments, but they were moderate to high in the SPM. Organic carbon partition coefficient values for HCH in this study were higher than previously published values and may reflect new input in this area. The residual HCHs in this area could be derived from a mixture of technical HCH and lindane because ongoing lindane use may be occurring. DDT in the majority of the study area was primarily attributed to historical discharge, but some regions may be receiving new input. The ecological risks of γ-HCH in the water were very low according to species sensitivity distribution models. The concentrations of HCH and DDT in the sediments from the study area did not exceed the sediment quality guidelines, which indicate little risk for benthic organisms.  相似文献   

5.
Concentrations of organochlorine pesticides (OCPs; dichlorodiphenyltrichloroethanes (DDTs), hexachlorocyclohexanes (HCHs), hexachlorobenzene (HCB)) were investigated in 105 soil samples collected in vicinity of the chemical industrial parks in Tianjin, China. OCP concentrations significantly varied in the study area, high HCH and DDT levels were found close to the chemical industrial parks. The intensity of agricultural activity and distance from the potential OCP emitters have important influences on the OCP residue distributions. Principal component analysis indicates that HCH pollution is a mix of historical technical HCH and current lindane pollution and DDT pollution input is only due to technical DDT sources. The significant correlations of OCP compounds reveal that HCHs, DDTs and HCB could have some similar sources of origin.  相似文献   

6.
Fourteen surface water and nine surface sediment samples were collected from the Peacock River and analyzed for organochlorine pesticides (OCPs) by gas chromatograph?Celectron capture detector (GC-ECD). All the analyzed organochlorine pesticides, except o,p ??-DDT, were detected in sediments from the Peacock River; but in the water samples, only ??-HCH, HCB, p,p ??-DDD, and p,p ??-DDT were detected at some sites. The ranges for total OCPs in the water and sediments were from N.D. to 195 ng l???1 and from 1.36 to 24.60 ng g???1, respectively. The only existing HCH isomer in the water, ??-HCH, suggested that the contamination by HCHs could be attributed to erosion of the weathered agricultural soils containing HCHs compounds. Composition analyses showed that no technical HCH, technical DDT, technical chlordanes, endosulfans, and HCB had been recently used in this region. However, there was new input of ??-HCH (lindane) into the Peacock River. The most probable source was water flowing from Bosten Lake and/or agricultural tailing water that was returned directly into the Peacock River. DDT compounds in the sediments may be derived mainly from DDT-treated aged and weathered agricultural soils, the degradation condition was aerobic and the main product was DDE. HCB in the sediment might be due to the input from Bosten Lake and the lake may act as an atmospheric deposition zone. There was no significant correlation between the concentrations of OCPs (including ??HCH, ??DDT, chlordanes, endosulfans, HCB and total OCPs) and the content of fine particles (<63 ??m). The concentrations of OCPs were affected by salinity.  相似文献   

7.
The Xiangjiang River (XR), the second largest tributary of the Yangtze River, is mainly located in Hunan province in south-central China. Nineteen surface sediment samples (the top 3-cm layer) collected from XR were analyzed to determine the concentrations, distribution, sources, and ecological risk of organochlorine pesticides (OCPs). The concentrations of OCPs were 3.0–29.8 ng/g (dry weight) with a mean of 12.6?±?7.7 ng/g. The widely detected compounds included HCHs, DDTs, HCB, and dieldrin. Overall, the dominant OCPs in the sediments were mainly composed of residual and degradation products, e.g., β-HCH with a mean of 42.2 % in HCHs and p,p′-DDE with a mean of 43.5 % in DDTs, implying that OCPs in the sediments had suffered from long-term aging without fresh inputs in XR. However, there was a high proportion of p,p′-DDT to DDTs in three sites, suggesting that there was use of technical DDT from their surrounding areas at present. The ratios of α-HCH/γ-HCH and p,p′-DDD?+?p,p′-DDE/DDTs increase from the upper reaches to the lower reaches of XR, suggesting sediments enriched with α-HCH and metabolites DDD and DDE during sediment transport process and could be attributed to the transformation of γ-HCH to α-HCH and DDT to DDE or DDD. The assessment of the ecological risk indicates that the OCPs in the sediments of XR have a moderate adverse biological effect on organisms.  相似文献   

8.
Organochlorine pesticides (OCPs) have variously been phased out in agricultural activities, but they are still widely detected in air, water, and soil systems due to their recalcitrant nature in the environment. The purposes of this study were to assess potential OCP pollution via dry and wet deposition over the fast developing Pearl River Delta area with 41,700 km2, where the main effort has been focused on emerging pollutants such as petroleum hydrocarbons and PM2.5. We quantified both the dry and wet deposition fluxes of 19 OCPs including dichlorodiphenyltrichloroethanes (DDTs), endosulfans (Endos), and hexachlorocyclohexanes (HCHs). The results showed that each year about 67.4, 42.0, 15.0, and 8.07 kg of total OCPs, DDTs, Endos, and HCHs were returned to the ground, among which 11.7, 10.4, 0.84, and 0.16 kg were in the dry deposition forms. The large spatial variations in OCP deposition fluxes indicated that OCP pollution in the air is mainly influenced on local scales because evaporation from local soil is likely the major source of the phased out OCPs. Source analysis indicated that DDTs may be still in use as antifouling agent and/or dicofol, but Endos and HCHs were mainly derived from the residual of historical usage. The study suggests that the historical OCP pollutants are persistent at high levels in this area and should not be overlooked, while we tackle emerging pollutants.  相似文献   

9.
The residues of 13 organochlorine pesticides (OCPs) in surface water and HCHs and DDTs in suspended particulate matter (SPM) from rivers and lakes in Yangtze River catchment of Wuhan, China, were investigated. The concentration of total OCPs in surface water varied from 1.01 to 46.49 ng l−1 (mean 10.55 ng l−1). The levels of total HCHs (ΣHCH) and total DDTs (ΣDDT) in surface water were in the range of 0.55–28.07 ng l−1 and lower than detection limit to 16.71 ng l−1, respectively, which was lower than Chinese standards on the whole. For OCPs residues in SPM, the mean levels varying from 0.20 to 34.72 ng l−1 and 0.46 to 2.72 ng l−1 for ΣHCH and ΣDDT, respectively, which ranked the relatively higher levels among Chinese studied rivers. Results from this investigation showed that previous excessive usage of technical OCPs was the main reason for the residues of HCHs and DDTs both in surface water and SPM, although some new sources were likely to occurred in the region. Apart from the OCPs in SPM originated from upstream in flood season, one of the important sources of OCP residues both in water and SPM in Yangtze River was supposed to be the inputs of its tributaries. Additionally, in situ water-SPM phase distributions of OCPs indicated that HCHs tended totransport with water as well as DDTs was prone to combine with SPM in Yangtze River catchment of Wuhan.  相似文献   

10.
The residues of organochlorine pesticides (OCPs) in 19 surface sediments of Bohai Sea Bay were determined in this study. Total OCP concentration in surface sediment ranged from 9.01 to 18.04 ng/g dry weight, with a mean concentration of 12.50 ng/g. These findings are in the mid-range of pesticide concentrations compared to those reported in other regions worldwide. DDTs and HCHs were the predominant species. The α-HCH/β-HCH ratios and the predominant γ-HCH indicate that the technical HCH contamination was due mainly to historical usage, although there appeared to be a fresh input of lindane. The results from \(\left( {\mbox{DDD}\,\mbox{+}\,\mbox{DDE}} \right)\mbox{/}\sum {\mbox{DDTs}} \) and DDD/DDE calculations suggest that the usage of DDT in agricultural activities was not terminated, and the historical/fresh inputs of DDT in these areas could be more easily degraded into DDD under an anoxic condition. PCA implies that the recent usage of DDT could serve as important fresh input sources for OCPs.  相似文献   

11.
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   

12.
The concentrations of 16 polycyclic aromatic hydrocarbons (PAHs) were determined by gas chromatography equipped with a mass spectrometry detector in 105 topsoil samples from an industrial area around Bohai Bay, Tianjin in the North of China. Results demonstrated that concentrations of PAHs in 104 soil samples from this area ranged from 68.7 to 5,590 ng g???1 dry weight with a mean of ∑16PAHs 814 ± 813 ng g???1, which suggests that there exists mid to high levels of PAH contamination. The concentration of ∑16PAHs in one soil sample from Tianjin Port was exceptionally high (48,700 ng g???1). Ninety-three of the 105 soil samples were considered to be contaminated with PAHs (>200 ng g???1), and 25 were heavily polluted (>1,000 ng g???1). The sites with high PAHs concentration are mainly distributed around chemical industry parks and near highways. Two low molecular weight PAHs, naphthalene and phenanthrene, were the dominant components in the soil samples, which accounted for 22.1% and 10.7% of the ∑16PAHs concentration, respectively. According to the observed molecular indices, house heating in winter, straw stalk combustion in open areas after harvest, and petroleum input were common sources of PAHs in this area, while factory discharge and vehicle exhaust were the major sources around chemical industrial parks and near highways. Biological processes were probably another main source of low molecular weight PAHs.  相似文献   

13.
Forty-nine superficial sediment samples used in this study were collected from eight sites in the Bahia Blanca Estuary, located in the Buenos Aires Province southwest, Argentina, in a period between April 2005 and March 2009, to assess the concentration levels, spatial and seasonal distribution, and putative input sources of 18 selected organochlorine pesticides (OCs), following UNEP-IAEA procedures. Average concentration levels in sediments ranged between 3.54 and 63.79 ng g???1, d.w. (mean = 15.99 ng g???1, d.w.), for ??OCs, and from nondetectable to 8.03 ng g???1, d.w. (mean = 2.16 ng g???1, d.w.), and from nondetectable to 3.20 ng g???1 (mean = 0.97 ng g???1, d.w.) for hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs), respectively. Principal component analysis allowed the classification of sampling sites according to the main OCs inputs over the estuary. In comparison to other worldwide locations and to the world coastal sediment concentrations range, sediment DDTs and HCHs levels were in the low range; on the opposite, ??OCs average was in the medium range. OCs seasonal distribution was found to be highly correlated with the precipitations seasonality and sowing seasons in the adjacent agriculture fields. In addition, an ecotoxicological risk assessment pointed industrial and agriculture catchment zones with intermediate probability of adverse effects to biota, while the city sewage outfall was classified with none indication of an immediate threat. Data indicated that the estuary sediments were functioning as a sink for persistent OC pesticides (either in use or banned), however, it was found a declining trend on their environmental burden.  相似文献   

14.
Tissue distribution and bioaccumulation of organochlorine pesticides (OCPs) in edible fishes collected from Taihu Lake, Cyprinus carpio (C. carpio) and Ctenopharyngodon idellus (C. idellus), were studied. OCPs were detected in all samples with hexachlorocyclohexanes (HCHs), aldrins (including aldrin, dieldrin, endrin, endrin aldehyde, and endrin ketone), heptachlors (heptachlor and heptachlor epoxide) and dichlorodiphenyltrichloroethanes (DDTs) being the predominant compounds for both fish species. Gill and gonad were found to be the dominant tissues for OCP bioaccumulation followed by liver, while muscle showed the least affinity of OCPs for both fishes. Tissue distribution indicated the exchange of contaminants between water and gill, as well as the food intake from environment were the dominant pathways for OCP bioaccumulation in gill-breathing fish, and the following tissue distribution was affected by both the physiological properties of target tissues and physicochemical characteristics of pesticides. OCP residues in fish were species-specific (45.63–1575.26 ng/g dry weight (dw) for C. idellus; 8.40–60.23 ng/g dw for C. carpio) mainly due to the growth rate of individuals as well as the metabolic capacity difference among species. HCHs and DDTs observed in fishes from Taihu Lake were comparable and moderate with other reported places in China. Human exposure risk assessment performed with the estimated daily intake values demonstrated the consumption of target fish species in Taihu Lake at present was safe.  相似文献   

15.
Eighty-two surface soil samples were collected from forest, grassland, tea estate, wildlife sanctuary, wetland, and roadside areas from the northeastern states of India, viz., Tripura, Manipur, and Assam. Thirteen different organochlorine pesticides (OCPs) were detected from background soils using gas chromatography electron capture detector. Manipur soils were found to be with higher concentration of dichlorodiphenyltrichloroethanes (DDTs), hexachlorocyclohexanes (HCHs), and endosulfan followed by Tripura and Assam. The spearman correlation coefficient shows significant correlation between HCHs, DDTs, and endosulfan isomers (r 2?>?0.5 and p?<?0.05). Additionally, α-HCH, δ-HCH, o,p′-DDE, and endosulfan-sulfate shows good correlation with total organic carbon in soil (r 2?=?0.5, p?=?0.05), indicating that the soil organic matter could enhance adsorption of these compounds, also demonstrating that the present OCPs in the background soil were from similar source. Further principal component analysis evaluates that most of the higher volatile compounds where clustered together in soil. However, after comparing with different states of Indian soil samples, the concentrations of OCPs in the present study areas are much lower and comparable with background soil across the globe.  相似文献   

16.
In this study, the semipermeable membrane device (SPMD) passive samplers were used to determine freely dissolved concentrations of polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in selected water bodies situated in and around Johannesburg City, South Africa. The devices were deployed for 14 days at each sampling site in spring and summer of 2011. Time weighted average (TWA) concentrations of the water-borne contaminants were calculated from the amounts of analytes accumulated in the passive samplers. In the area of interest, concentrations of analytes in water ranged from 33.5 to 126.8 ng l?1 for PAHs, from 20.9 to 120.9 pg l?1 for PCBs and from 0.2 to 36.9 ng l?1 for OCPs. Chlorinated pesticides were mainly composed of hexachlorocyclohexanes (HCHs) (0.15–36.9 ng l?1) and dichlorodiphenyltrichloromethane (DDT) with its metabolites (0.03–0.55 ng l?1). By applying diagnostic ratios of certain PAHs, identification of possible sources of the contaminants in the various sampling sites was performed. These ratios were generally inclined towards pyrogenic sources of pollution by PAHs in all study sites except in the Centurion River (CR), Centurion Lake (CL) and Airport River (AUP) that indicated petrogenic origins. This study highlights further need to map up the temporal and spatial variations of these POPs using passive samplers.  相似文献   

17.
The aim of this study was to evaluate the consequence of changing land use from agriculture land to other use purposes with respect to OCPs non-cancer and cancer risk on human health, based on concentrations of DDTs and HCHs in soils collected from 55 locations representing 12 different land use types. There were no non-cancer risks of DDTs and γ-HCHs on adults and children, and there were very low cancer risks of DDD, o,p'-DDE, DDT, α-HCH, β-HCH, γ-HCH based on their total concentrations in all samples. Nonetheless, there were significant correlations of DDT to its metabolites (DDE and DDD) (r = 0.506 and r = 0.648) and DDE to DDD (r = 0.438) both at p < 0.01. OCP levels should be routinely monitored in different environmental media and food in order to verify whether there is fresh input. Their potential risks on human health should also be assessed.  相似文献   

18.
Organochorine (OCs) residues were measured in human breast milk samples from four Tunisian women. Month-mix samples composed of weekly collected breast milk samples were analyzed over the lactation period between 3 days after delivery and 10 months post-partum. The concentrations of dichlorodiphenytrichloroethane and its metabolites (DDTs), hexachlorobenzene (HCB), hexachlorocyclohexane isomers (HCHs), dieldrin, and 20 polychlorinated biphenyl congeners (PCBs) were determined by gas chromatography with electron capture detection. The variation of OC residue levels in human milk was investigated for each woman individually. The average p,p’-DDE and p,p’-DDT concentrations declined from 661- and 438-ng g?1 fat basis at day 3 to 77- and 106-ng g?1 fat basis after 8 months, respectively. No essential changes in HCB, HCHs, dieldrin, and total PCBs concentrations in human breast milk occurred over the lactation periods investigated; the concentrations remained either relatively constant or show no significant weak decrease.  相似文献   

19.
The analyses of environmentally persistent pollutants like polychlorinated biphenyls (PCBs), hexachlorocyclohexane (HCH) isomers, and dichlorodiphenyltrichloroethane (DDT) and its metabolites in surficial sediment samples collected from 17 locations along with the coast of the Red Sea in Egypt were carried out using gas chromatography–mass spectrometry. Several potential organic contaminants from agricultural (e.g., DDT and its breakdown products, lindane, endrin, dieldrin, and endosulfan) and industrial (PCBs) sources were measured. The levels of 20 organochlorine pesticides (OCPs) and ten PCB congeners in sediment collected from 17 stations along ~1,200 km were investigated. Concentrations of PCBs, HCHs, DDTs, and cyclodienes ranged from 0.40 to 6.17, 0.01 to 0.09, n.d. to 0.46, and 0.08 to 0.90 ppb dry weight. Two statistical programs were applied on the data (principal component analysis, PCA, and cluster analysis, CA), and it was concluded that it is impossible to predict the distribution patterns of the OCPs in a contaminated area. Risk assessment of the organochlorines contaminated in the sediments of the studied area was investigated.  相似文献   

20.
Blue mussels (Mytilus edulis) and sediments collected from 1991 to 2005 from New Bedford Harbor (NBH), MA, were analyzed for two polycyclic musks (HHCB or Galaxolide® and AHTN or Tonalide®), polybrominated diphenyl ethers (PBDEs), polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OCPs). HHCB and AHTN were found in mussel tissues at mean concentrations of 836 and 376 ng/g lipid weight (lw), respectively, which were two- to seven-fold higher than those found at a reference site. Mean concentrations of HHCB and AHTN in NBH sediments were 12 and 6.3 ng/g dry weight (dw), respectively. Four- and five-ringed PAHs, such as phenanthrene, anthracene, fluoranthene, and pyrene, collectively accounted for 61 % of the ∑PAHs concentrations in mussels from NBH. Mean ΣPCB concentrations in mussels from upper and lower NBH were 942 and 182 μg/g lw, respectively, and were dominated by tetra- and penta-chlorobiphenyl congeners, collectively accounting for 61 % of the ΣPCB concentrations. The mean concentration of ∑PBDEs in mussels from NBH was 277 ng/g lw, and no significant difference existed in the concentrations between upper and lower NBH. DDTs were the major OCP found in mussels, found at a mean concentration of 778 ng/g lw. The concentrations of HHCB, AHTN, ΣPBDEs, ΣPAHs, and DDTs in mussels decreased significantly (r 2?≥?0.56, p?≤?0.052) from 1991 to 2005. The concentrations of PCBs and chlordanes did not exhibit a decreasing trend in mussel tissues (r 2?<?0.50; p?>?0.076) from 1991 to 2005. Based on the temporal trends in the concentrations of HHCB, AHTN, ∑PAHs, and ∑PBDEs found in mussels from NBH, it was estimated that between 5.5 and 12 years were required for the concentrations of these compounds to decrease by half (i.e., environmental halving time) of the levels found in 1991.  相似文献   

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