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1.
We determined the concentrations of 35 PCNs, 12 PCBs, and 20 PAHs in 49 urban topsoils under different land use (house garden, roadside grassland, alluvial grassland, park areas, industrial sites, agricultural sites) and in nine rural topsoils. The sums of concentrations of 35 PCNs (sigma35 PCNs) were <0.1-15.4 microg kg(-1) in urban soils and <0.1 to 0.82 microg kg(-1) in rural soils. The PCN, PCB, and PAH concentrations were highest at industrial sites and in house gardens. While rural soils receive PCNs, PCBs, and PAHs by common atmospheric deposition, there are site-specific sources of PCNs, PCBs, and PAHs for urban soils such as deposition of contaminated technogenic materials. The PCN, PCB, and PAH concentrations decreased from the central urban to the rural area. In the same order the contribution of lower chlorinated PCNs and PCBs increased because they are more volatile and subject to increased atmospheric transport. The PCNs 52+60, and 73 were more abundant in soil samples than in Halowax mixtures, indicating that combustion contributed to the PCN contamination of the soils.  相似文献   

2.
We determined 20 polycyclic aromatic hydrocarbons (PAHs) and 12 polychlorinated biphenyls (PCBs) in Oi, Oe, and Oa horizons and at 0-5 and 15-20 cm mineral soil depth of 16 Norway spruce (Picea abies) stands in north Bavaria. The sum of PAH concentrations increased along the line Oi (mean+/-SD: 841+/-330 microg kg(-1))相似文献   

3.
Persistent organic pollutants (PAHs and PCBs) in soil samples from seven sites across the Seine basin were analysed. Samples were taken from industrialized, urban, suburban and remote sites. Results showed spatial differences, in terms of concentrations and congener profiles. PAH (Sigma14 PAHs) and PCB (Sigma 7 PCBs) concentrations ranged from 450 to 5650 microg kg(-1) and 0.09 to 150 microg kg(-1), respectively. A clear gradient from industrial to remote sites was highlighted, with a ratio of up to one order of magnitude for PAHs and two orders of magnitude for PCBs. Fluoranthene and pyrene were predominant, while the carcinogenic PAHs represented 15-46% of the total PAH content. Using hierarchical cluster analysis, soil samples profiles were compared and the influence of site location and potential sources were identified: automobile traffic, domestic heating, and industrial emissions were the prevalent PAHs sources in the Seine basin. PCB profiles suggested different transport patterns among congeners. For remote sites, the congener fingerprint showed a relatively higher proportion of the most volatile congeners, which were attributed to increased atmospheric residence times. Thus, PAH and PCB distributions in soils provided information on sources and evidence for short-range transport, and profiles of compounds reflected differences between regional and local emissions. This study demonstrates that soil sampling can be used to investigate spatial differences in atmospheric inputs of persistent organic pollutants based on differences in the mixtures of compounds, reflecting differences in regional and local atmospheric emissions.  相似文献   

4.
Yang Y  Ligouis B  Pies C  Achten C  Hofmann T 《Chemosphere》2008,71(11):2158-2167
Organic petrographic analysis was applied to provide direct information on carbonaceous geosorbents for PAHs in river floodplain soils. The anthropogenic OM group (primarily coal and coal-derived particles) displayed large volume amounts for all the soil samples. Distinct PAH concentrations with similar PAH distribution patterns were determined in grain size and density fractions for each sample. Two-ring PAHs had stronger correlation to organic carbon (OC) than black carbon (BC) contents, while heavier PAHs showed correlation to BC, rather than OC. In this study, we combined grain size and density separation, PAH determinations, TOC and BC measurements, and organic petrographic identification, and concluded that two-ring PAHs in soils were associated to coal particles. Other heavier PAHs could be more controlled by black carbon (BC), which were mostly coal-derived particles from former coal mining and coal industrial activity.  相似文献   

5.
Persistent Organic Pollutants (POPs) and Polycyclic Aromatic Hydrocarbons (PAHs) are important classes of compounds of serious environmental concern. These compounds were measured in waters, sediments and soils from several high altitude sites in the Sagarmatha National Park (Nepal) and included in the Himalayan ridge.In water samples, low-level substituted PCBs and PBDEs, along with more volatile PAHs, were the most common contaminants. In sediment and soil samples, the PCB profile was mainly composed of medium-level chlorinated congeners and significantly correlated with altitude. The PAH profile for water and soil samples showed the main contribution of pyrogenic PAHs due to emissions of solid combustion, whereas the profile for sediments indicated the main contribution of pyrogenic PAHs from gasoline emissions. The PAH levels measured in Himalayan samples must be considered as low to medium contaminated, whereas the regarded Himalayan stations can be considered undisturbed remote areas concerning PCB, PBDE and OC compounds.  相似文献   

6.
BACKGROUND, AIM, AND SCOPE: Polycyclic aromatic hydrocarbons (PAHs) are widespread environmental contaminants and contribute to the pollution of soil environment. Soil ingestion is of increasing concern for assessing health risk from PAH-contaminated soils because soil ingestion is one of the potentially important pathways of exposure to environmental pollutants, particularly relevant for children playing at contaminated sites due to their hand-to-mouth activities. In vitro gastro-intestinal tests imitate the human digestive tract, based on the physiology of humans, generally more simple, less time-consuming, and especially more reproducible than animal tests. This study was conducted to investigate the level of PAH contamination and oral bioaccessibility in surface soils, using physiologically based in vitro gastro-intestinal tests regarding both gastric and small intestinal conditions. MATERIALS AND METHODS: Wastewater-irrigated soils were sampled from the metropolitan areas of Beijing and Tianjin, China, which were highly contaminated with PAHs. Reference soil samples were also collected for comparisons. At each site, four soils were sampled in the upper horizon at the depth of 0-20 cm randomly and were bulked together to form one composite sample. PAH concentrations and origin were investigated and a physiologically based in vitro test was conducted using all analytical grade reagents. Linear regression model was used to assess the relationship between total PAH concentrations in soils and soil organic carbon (SOC). RESULTS: A wide range of total PAH concentrations ranging from 1,304 to 3,369 mug kg(-1) in soils collected from different wastewater-irrigated sites in Tianjin, while ranging from 2,687 to 4,916 mug kg(-1) in soils collected from different wastewater-irrigated sites in Beijing, was detected. In general, total PAH concentrations in soils from Beijing sites were significantly higher than those from Tianjin sites, indicating a dominant contribution from both pyrogenic and petrogenic sources. Results indicated that the oral bioaccessibility of PAHs in small intestinal was significantly higher (from P < 0.05 to P < 0.001) than gastric condition. Similarly, the oral bioaccessibility of PAHs in contaminated sites was significantly higher (from P < or = 0.05 to P < 0.001) than in reference sites. Individual PAH ratios (three to six rings), a more accurate and reliable estimation about the emission sources, were used to distinguish the natural and anthropogenic PAH inputs in the soils. Results indicated that PAHs were both pyrogenic and petrogenic in nature. DISCUSSION: The identification of PAH sources and importance of in vitro test for PAH bioaccessibility were emphasized in this study. The oral bioaccessibility of individual PAHs in soils generally decreased with increasing ring numbers of PAHs in both the gastric and small intestinal conditions. However, the ratio of bioaccessibility of individual PAHs in gastric conditions to that in the small intestinal condition generally increased with increasing ring numbers, indicating the relatively pronounced effect of bile extract on improving the bioaccessibility of PAHs with relatively high ring numbers characterized by their high K ( ow ) values. Similarly, total PAH concentrations in soils were strongly correlated with SOC, indicating that SOC was the key factor determining the retention of PAHs in soils. CONCLUSIONS: Soils were contaminated with PAHs due to long-term wastewater irrigation. PAHs with two to six rings showed high concentrations with a significant increase over reference soils. Based on the molecular indices, it was suggested that PAHs in soils had both pyrogenic and petrogenic sources. It was also concluded that the oral bioaccessibility of total PAHs in the small intestinal condition was significantly higher than that in the gastric condition. Furthermore, the bioaccessibility of individual PAHs in soils generally decreased with the increasing ring numbers in both the gastric and small intestinal conditions. RECOMMENDATIONS AND PERSPECTIVES: It is suggested that more care should be given while establishing reliable soil criteria for PAHs, especially concerning the health of children who may ingest a considerable amount of PAH-contaminated soil via outdoor hand-to-mouth activities.  相似文献   

7.
Hydrophobic organic contaminants (HOC) (i.e. PAHs and PCBs) were measured in the water column and in Eurytemora affinis samples from the Seine Estuary collected from November 2002 to February 2005. Results showed seasonal variations of both total PCB and PAH levels in the suspended particulate matter (SPM) and in the copepods with maximum levels during winter times. PAH and PCB concentrations in the SPM ranged from 499 to 5819ngg(-1) and from 58 to 463ngg(-1), respectively. Phenanthrene, pyrene and benzo[b+j+k]fluoranthene (B[b+j+k]F) were the predominant PAH compounds in the water column, while CB 101, 118, 153 and 138 were the most abundant PCB congeners. PCBs and PAHs bioaccumulated by E. affinis (EA) varied between 383 and 1785ngg(-1) and 165-3866ngg(-1). CB101, 153, 138 and B[b+j+k] were, respectively, the major compounds of PCB and PAH fingerprints in EA. Thereby, the copepods could reach high accumulation factor (ACF) (91000 for PCBs and 17000 for PAHs). The principal component analyses of contaminant concentrations and environmental parameter datasets distinguished two groups of copepods. The winter time cluster, with high percentage of adult copepods, which bioaccumulated the highest PCB and PAH body-burdens, and the second cluster with juveniles showing the lowest HOC concentrations. Thus, PAH and PCB concentrations in EA exhibited significant correlations with the percentage of adults making up the samples.  相似文献   

8.
Distributions and concentrations of PAHs in Hong Kong soils   总被引:19,自引:0,他引:19  
Surface soil (0-10 cm) samples from 53 sampling sites including rural and urban areas of Hong Kong were collected and analyzed for 16 EPA priority polycyclic aromatic hydrocarbons (PAHs). Total PAH concentrations were in the range of 7.0-410 microg kg(-1) (dry wt), with higher concentrations in urban soils than that in rural soils. The three predominant PAHs were Fluoranthene, Naphthalene and Pyrene in rural soils, while Fluoranthene, Naphthalene and Benzo(b + k)fluoranthene dominated the PAHs of urban soils. The values of PAHs isomer indicated that biomass burning might be the major origin of PAHs in rural soils, but vehicular emission around the heavy traffic roads might contribute to the soil PAHs in urban areas. A cluster analysis was performed and grouped the detectable PAHs under 4 clusters, which could be indicative of the PAHs with different origins and PAHs affected by soil organic carbon contents respectively.  相似文献   

9.
A PAH contaminated river floodplain soil was separated according to grain size and density. Coal and coal-derived particles from coal mining, coal industry and coal transportation activities were identified by organic petrographic analysis in our samples. Distinct concentrations of PAHs were found in different grain size and density fractions, however, similar distribution patterns of PAHs indicated similar sources. In addition, although light fractions had the mass fraction by weight of less than 5%, they contributed almost 75% of the total PAHs in the soil. PAH concentrations of all sub fractions showed positive correlation with their TOC contents. Altogether, coal and coal-derived particles that were abundant in light fractions could be the dominant geosorbents for PAHs in our samples.  相似文献   

10.
Distributions of total organic carbon (TOC), black carbon (BC), and polycyclic aromatic hydrocarbons (PAH) were investigated in different particle size fractions for four Norwegian harbor sediments. The total PAH (16-EPA) concentrations ranged from 2 to 113 mg/kg dry weight with the greatest fraction of PAH mass in the sand fraction for three of the four sediments. TOC contents ranged from 0.84% to 14.2% and BC contents from 0.085% to 1.7%. This corresponds to organic carbon (OC = TOC - BC) contents in the range of 0.81-14% and BC:TOC ratios of 1.3-18.1%. PAH isomer ratios suggested that the PAH in all four sediments were of pyrogenic origin. Furthermore, stronger correlations between PAH versus BC (r2 = 0.85) than versus OC (r2 = 0.15) were found. For all size fractions and bulk sediments, the PAH-to-BC ratios for the total PAHs were on average 6+/-3 mg PAH/g BC. These results suggest that PAH distributions were dominated by the presence of BC, rather than OC. As sorption to BC is much stronger than sorption to OC, this may result in significantly lower dissolved concentrations of PAH than expected on the basis of organic carbon partitioning alone.  相似文献   

11.
In soils of the Moscow region, we examined PCB concentrations in bulk samples and aggregate fractions. Topsoils under grassland and forest at five locations along a southeast-bound transect from Moscow and at a northeastern background location (grassland only) were analysed. We collected aggregates >1 cm and fractionated them into interior and exterior portions and also analysed the remaining soil without the aggregates >1 cm. The concentrations of the sum of 17 PCBs (sigma17PCBs) in 35 bulk soil samples ranged from 3.1 to 42 microg kg(-1). This was 48-61% of the sigma33PCBs determined in 23 selected samples. The congeners 138(+158), 101 and 52 were most abundant. All PCB concentrations and the degree of chlorination declined with increasing distance from Moscow. The PCBs were accumulated in the aggregate exterior (on average 146% of the sigma17PCBs in bulk soil). We conclude that the ecotoxicological risk of PCBs in soils may not be properly assessed with the conventional bulk soil analysis.  相似文献   

12.
Zohair A  Salim AB  Soyibo AA  Beck AJ 《Chemosphere》2006,63(4):541-553
The residues of polyaromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in soils from organic farms and their uptake by four varieties of organic-produced potatoes and three varieties of organic carrots from England were investigated. Samples of the soils, crop peels and cores were all Soxhlet-extracted in triplicate, cleaned up by open-column chromatography and analysed by a multi-residue analytical method using gas chromatography with mass selective detection. The concentrations of PAHs, PCBs and OCPs in soils from organic farms ranged from 590+/-43 to 2301+/-146 microg/kg, 3.56+/-0.73 to 9.61+/-1.98 microg/kg and 52.2+/-4.9 to 478+/-111 microg/kg, respectively. Uptake by different crop varieties were 8.42+/-0.93 to 40.1+/-4.9 microg/kg sigmaPAHs, 0.83+/-0.19 to 2.68+/-0.94 microg/kg sigmaPCBs and 8.09+/-0.83 to 133+/-27 microg/kg sigmaOCPs. Residue uptake from soils depended on plant variety; Desiree potato and Nairobi carrot varieties were more susceptible to PAH contamination. Likewise, uptake of PCBs and OCPs depended on potato variety. There were significant positive correlations between the PCB and OCP concentrations (P<0.05) in soils and carrots but no significant correlation was found between the concentrations of any contaminants in soils and potatoes. Peeling carrots and potatoes was found to remove 52-100% of the contaminant residues depending on crop variety and the properties of the contaminants. Soil-crop bioconcentration factors (BCFs) decreased with increasing logK(ow) for PAHs up to about 4.5 and for PCBs up to about 6.5, above which no changes were discernible for either class of contaminants. No relationship was observed between soil-crop BCFs and logK(ow) for OCPs, most likely because their concentrations were low and variable.  相似文献   

13.
Earlier studies had shown significant differences in sorption of nine pesticides in soils collected from two landuses (native vegetation and market gardens), which could not be explained on the basis of organic carbon content alone. Consequently it was hypothesised that the differences in sorption behaviour between the two landuses may be due to variation in the chemistry of the organic carbon. In this study the relationship between sorption behaviour of the nine chemicals and soil organic carbon chemistry, as determined by solid-state (13)C NMR spectroscopy, was investigated. No significant differences were found between the two landuses in the distribution of the four main spectral regions of the (13)C NMR spectra of soil OC, except for the carbonyl fraction (165-220ppm), which may reflect the low OC content of the soils from both landuses. For all chemicals, except prometryne, the most significant (P<0.01 or P<0.001) relationship between K(d) values and types of OC was found with the aromatic (110-165ppm) or the alkyl (0-45ppm) fraction. A comparison was made of the variability of K(d) values normalized over OC (i.e. K(oc)), alkyl, aromatic and alkyl+aromatic fractions. Expressing K(d) values for all chemicals, except azinphos methyl, in soils under native vegetation as K(alkyl) or K(aromatic) greatly decreased the variability compared with the K(oc) value. However in the cultivated soils only the sorption coefficients for DEA, DIA and fenamiphos showed a decrease in variability when expressed as K(alkyl) or K(aromatic). This reflected the stronger relationship between sorption coefficients and the alkyl and aromatic fraction of soil OC in soils from native vegetation compared with those determined from the market garden soils. The different relationships between sorption coefficients and types of OC of the two landuses also suggests that the type of aromatic and alkyl carbon under the two landuses is different and NMR characterisation of the OC was not sufficient to distinguish these differences.  相似文献   

14.
Hong L  Luthy RG 《Chemosphere》2008,72(2):272-281
Polyoxymethylene (POM) is a polymeric material used increasingly in passive sampling of hydrophobic organic contaminants such as PAHs and PCBs in soils and sediments. In this study, we examined the sorption behavior of 12 PAH compounds to POM and observed linear isotherms spanning two orders of magnitude of aqueous concentrations. Uptake kinetic studies performed in batch systems for up to 54 d with two different volume ratios of POM-to-aqueous phase were evaluated with coupled diffusion and mass transfer models to simulate the movement of PAHs during the uptake process and to assess the physicochemical properties and experimental conditions that control uptake rates. Diffusion coefficients of PAHs in POM were estimated to be well correlated with diffusants' molecular weights as D(POM) proportional, variant(MW)(-3), descending from 2.3 x 10(-10) cm(2) s(-1) for naphthalene to 7.0 x 10(-11) cm(2) s(-1) for pyrene. The uptake rates for PAHs with log K(ow)<5.8 were controlled by the POM phase and the hydrophobicity of PAH compounds. For more hydrophobic PAH compounds, the aqueous boundary layer played an increasingly important role in determining the overall mass transfer rate. The POM partitioning technique was demonstrated to agree well with two other procedures for measuring PAH soil-water distribution coefficients in oil-soot (lampblack) containing soil samples.  相似文献   

15.
Honda K  Mizukami M  Ueda Y  Hamada N  Seike N 《Chemosphere》2007,68(9):1763-1771
The residue level of 21 polycyclic aromatic hydrocarbons (PAHs) and the temporal changes in this level were investigated in paddy soils collected from particular experimental sites in Japan from 1959 to 2002. The average total PAH concentration in all the samples was 496 microg kg(-1), and it ranged from 52.9 to 2180 microg kg(-1). The residue level of the PAHs was the highest during the 1960s, rapidly decreased during the 1970s, and remained almost constant thereafter. Relatively high PAH concentrations were observed in soils from areas that experienced heavy snowfall and that had relatively low air temperature. The predominant PAHs were phenanthrene, fluoranthene, naphthalene, and pyrene, and their concentration overall and in relation to that of the total PAHs decreased each year since the 1960s. Similarities in the PAH profiles among the locations were determined using the concentration correlation matrix and cluster analysis, and ratios of the levels of specific PAH pairs were also calculated to determine their origin. The collected data suggested that the origins of soil PAHs changed chronologically from the burning of agricultural wastes such as stubble before the mid-1970s to the combustion of fossil fuel and its secondary products after the mid-1970s.  相似文献   

16.
In this study the levels and distribution of some persistent toxic substances (PTS) were investigated in soils, superficial water, and snow along an altitudinal gradient in the Laja River Basin (South Central Chile). The principal objective was to establish the basin's contamination status. The working hypothesis was that PTS levels and distribution in the basin are dependent on the degree of anthropogenic intervention. Fifteen PAHs, seven PCBs congeners, and three organochlorine pesticides were studied in superficial soil and water samples obtained along the altitudinal gradient and from a coastal reference station (Lleu-Lleu River). Soil samples were extracted using accelerated solvent extraction with acetone/cyclohexane (1:1) for PAHs and organochlorine compounds. Contaminants were extracted from water and snow samples by liquid-liquid extraction (LLE). PAH and organochlorine compound quantification was carried out by HPLC with fluorescence detection and GC-MS, respectively. PCBs in soils presented four different profiles in the altitudinal gradient, mainly determined by their chlorination degree; these profiles were not observed for the chlorinated pesticides. In general, the detected levels for the analyzed compounds were low for soils when compared with soil data from other remote areas of the world. Higher summation operator PAHs levels in soils were found in the station located at 227 masl (4243 ng g-1 TOC), in a forestry area and near a timber industry, where detected levels were up to eight times higher than the other sampling sites. In general, PAH levels and distribution seems to be dependent on local conditions. No pesticides were detected in surface waters. However, congeners of PCBs were detected in almost all sampling stations with the highest levels being found in Laja Lake waters, where 1.1 ng/l were observed. This concentration is two times higher than values reported for polluted lakes in the Northern Hemisphere. The presence of organochlorine compound in snow sampled at the highest elevation point of the basin is indicative of the transport and atmospheric deposition phenomena of alpha-HCH, gamma-HCH and PCB 52, with values being similar to the levels reported in Canadian snow samples. We conclude that environmental PTS substance levels are in general relatively low, although PAHs may be of concern in some areas of the basin.  相似文献   

17.
Song YF  Wilke BM  Song XY  Gong P  Zhou QX  Yang GF 《Chemosphere》2006,65(10):1859-1868
A study was carried out on the residue level of major concern pollutants (PAHs, PCBs and HMs) and the assessment of their genotoxicity in soils obtained from Shenyang, northeast of China which had been subjected to wastewater irrigation for more than 40 years. Topsoils (0-20cm) in paddy fields were sampled along the upper, middle and lower reaches of the wastewater disposal channel. Sixteen USEPA PAHs were determined by High Performance Liquid Chromatography (HPLC) with fluorescence detector, eight PCBs were detected by Gas Chromatography (GC) with electron capture detector, and six heavy metals (Cd, Cu, Pb, Zn, Ni, and Cr) were measured by Atomic Absorption Spectrophotometer (AAS). The genotoxicity effect of soils was examined by Vicia faba micronucleus (MN) test. Archived soils that had undergone a similar history of wastewater irrigation provided by Technical University of Berlin, Germany were subjected to analysis of the above pollutants and Vicia faba/MN test for comparison. Results indicated elevated residues of the studied pollutants (PAHs, especially benzo (a) pyrene, the eight PCB congeners and heavy metals) in both tested and archived soils. The MN frequencies were 2.2-48.4 times higher compared with the control. However, there was no correlation between the MN frequencies and the concentration of pollutants detected. This investigation suggested a potential ecological risk even with a lower level of residual pollutants in soil matrix after long-term wastewater irrigation.  相似文献   

18.
Soil and sediment samples from James Ross Island were analyzed for their PCB, OCP and PAH contents. Soil concentrations ranged between 0.51 and 1.82 ng g(-1) for seven indicator PCB congeners, between 0.49 and 1.34 ng g(-1) for HCH congeners, between 0.51 and 3.68 ng g(-1) for the sum of p,p'-DDT, DDE, and DDD, and between 34.9 and 171 ng g(-1) for the sum of 16 EPA PAHs. Sediment levels from 0.32 to 0.83 ng g(-1) were found for PCBs, from 0.14 to 0.76 ng g(-1) for HCHs, from 0.19 to 1.15 ng g(-1) for DDTs, and from 1.4 to 205 ng g(-1) for PAHs. A prevalence of low-mass PAHs, less chlorinated PCBs, and more volatile chemicals indicates that the long-range atmospheric transport from populated areas of Africa, South America, and Australia is the most probable contamination source for the solid matrices in James Ross Island.  相似文献   

19.
20.
Wang Y  Luo CL  Li J  Yin H  Li XD  Zhang G 《Chemosphere》2011,85(3):344-350
This study aimed at identifying the levels of PCBs generated from e-waste recycling, and their potential impacts on the soils and vegetations as well. The ΣPCBs concentrations in soil and plant samples ranged from 7.4 to 4000 ng g(-1) and from 6.7 to 1500 ng g(-1), respectively. For the plant samples, Chrysanthemum coronarium L. from vegetable field and the wild plant Bidens pilosa L. from the burning site showed relatively higher PCB concentrations than other species. For the soil samples, the e-waste burning site had relatively higher PCB concentrations than the adjacent areas, and vegetable soils had higher PCB concentrations than paddy soils. The PCB concentrations showed a clear decreasing trend with the increasing distance from the e-waste recycling site. PCB 28, 99, 101, 138, 153, and 180 were the predominant congeners. Principal component analysis results showed a potential fractionation of PCB compositions from the burning site to the surroundings. The PCB congener pattern at the burning site was similar to Arochlor 1260, pointing to an input of non-domestic e-waste. Similar PCB congeners were found in soils and related vegetables, indicating they derived from the same source. The consumption of vegetables grown in soils near e-waste recycling sites should be strictly avoided due to the high PCBs in the plant tissues.  相似文献   

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