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1.
Air samples collected in the German part of the North Sea from March to July 2010 were investigated for organophosphorus compounds (OPs) being applied as flame retardants and plasticizers. The ∑8OPs concentration ranged from 110 to 1400 pg m−3 while tris(2-chloroisopropyl) phosphate (TCPP) dominated all samples with individual concentrations up to 1200 pg m−3. The highest concentrations were observed in continental air masses showing the high influence of industrialized regions including production sites on atmospheric emissions and concentrations. The occurrence of OPs even in oceanic/Arctic air masses shows that OPs can undergo long-range atmospheric transport. Dry particle-bound deposition fluxes from 9 to 240 ng m−2 d−1 for ∑8OPs were estimated leading to a minimum annual flux of 710 ± 580 kg y−1 OPs into the German North Sea. This study presents the first occurrence of OPs in the marine atmosphere together with important information on their long-range transport potential.  相似文献   

2.
Contaminated sediments in the St. Lawrence River remain a difficult problem despite decreases in emissions. Here, sediment and pore water phases were analyzed for total mercury (THg) and methyl mercury (MeHg) and diffusion from the sediment to the overlying water was 17.5 ± 10.6 SE ng cm−2 yr−1 for THg and 3.8 ± 1.7 SE ng cm−2 yr−1 for MeHg. These fluxes were very small when compared to the particle-bound mercury flux accumulating in the sediment (183 ± 30 SE ng cm−2 yr−1). Studies have reported that fish from the westernmost site have higher Hg concentrations than fish collected from the other two sites of the Cornwall Area of Concern, which could not be explained by differences in the Hg flux or THg concentrations in sediments, but the highest concentrations of sediment MeHg, and the greatest proportions of MeHg to THg in both sediment and pore water were observed where fish had highest MeHg concentrations.  相似文献   

3.
Twenty precipitation samples were taken concurrently with air samples at a northern German monitoring site over a period of 7 months in 2007 and 2008. Thirty four poly- and perfluorinated compounds (PFC) were determined in rain water samples by solid phase extraction and HPLC-MS/MS analysis. Seventeen compounds were detected in rain water with ΣPFC concentrations ranging from 1.6 ng L−1 to 48.6 ng L−1. Perfluorooctanoate (PFOA) and perfluorobutanate (PFBA) were the compounds that were usually observed in highest concentrations. Calculated ΣPFC deposition rates were between 2 and 91 ng m−2 d−1. These findings indicate that particle phase PFC are deposited from the atmosphere by precipitation. A relationship between PFC wet deposition and air concentration may be established via precipitation amounts. Trajectory analysis revealed that PFC concentration and deposition estimates in precipitation can only be explained if a detailed air mass history is considered.  相似文献   

4.
Measurements of gaseous elemental mercury (GEM), particulate mercury (Hgp), and reactive gaseous mercury (RGM) were concurrently recorded at an urban site in Detroit and a rural site in Dexter, both in Michigan for the calendar year 2004. Their average concentrations (±standard deviation) for the urban area were 2.5 ± 1.4 ng m?3, 18.1 ± 61.0 pg m?3, and 15.5 ± 54.9 pg m?3, respectively, while their rural counterparts were 1.6 ± 0.6 ng m?3, 6.1 ± 5.5 pg m?3, and 3.8 ± 6.6 pg m?3, respectively. The medians of urban-to-rural ratios of Hg concentrations indicate approximately 1-fold, 2-fold, and 3-fold gradients between Detroit and Dexter for GEM, Hgp, and RGM, respectively. The urban–rural differences in Hg also varied considerably on different temporal scales and with wind flow patterns, which was most evident in RGM. Our results show that while Hg at both sites was impacted by regional sources, meteorological conditions, and photochemical transformations, the extent of variations in the observed urban-to-rural gradients, particularly in RGM, cannot be fully accounted for by these processes. Both analyses of the annual data and case studies indicate that the more variable and episodic nature of Hg, particularly RGM, seen in Detroit compared with Dexter, was the result of direct impact from local anthropogenic sources.  相似文献   

5.
Hou L  Liu M  Ding P  Zhou J  Yang Y  Zhao D  Zheng Y 《Chemosphere》2011,83(7):917-924
This study investigated the effects of sediment dewatering on the phosphorus transformations concerning about the production and emission of phosphine in the intertidal marsh of the Yangtze Estuary. The concentrations of matrix-bound phosphine ranged from 18.62-72.53 ng kg−1 and 31.14-61.22 ng kg−1 within the August and January exposure incubations, respectively. The responses of matrix-bound phosphine concentrations to sediment dessication demonstrate that the production (or accumulation) of matrix-bound phosphine significantly increased with water loss at the start of the emersion incubations. However, further dehydration inhibited the formation of matrix-bound phosphine in sediments. The significant correlations of matrix-bound phosphine with the organic-P bacteria abundance and alkaline phosphatase activities implicate that the production of matrix-bound phosphine within the dessication incubations was linked closely to the microbial decomposition of organic P. The emissions of phosphine generally decreased with sediment dewatering, with the fluxes of 7.51-96.73 ng m−2 h−1 and 5.34-77.74 ng m−2 h−1 over the exposure incubations of both August and January, respectively. Also, it is observed that the releases of phosphine during the entire exposure periods were affected not only by its production but also by sediment water and redox conditions.  相似文献   

6.
Probabilistic material flow analysis and graph theory were combined to calculate predicted environmental concentrations (PECs) of engineered nanomaterials (ENMs) in Swiss rivers: 543 river sections were used to assess the geographical variability of nano-TiO2, nano-ZnO and nano-Ag, and flow measurements over a 20-year period at 21 locations served to evaluate temporal variation. A conservative scenario assuming no ENM removal and an optimistic scenario covering complete ENM transformation/deposition were considered. ENM concentrations varied by a factor 5 due to uncertain ENM emissions (15%-85% quantiles of ENM emissions) and up to a factor of 10 due to temporal river flow variations (15%-85% quantiles of flow). The results indicate highly variable local PECs and a location- and time-dependent risk evaluation. Nano-TiO2 median PECs ranged from 11 to 1′623 ng L−1 (conservative scenario) and from 2 to 1′618 ng L−1 (optimistic scenario). The equivalent values for nano-ZnO and nano-Ag were by factors of 14 and 240 smaller.  相似文献   

7.
The residual levels of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere and in dissolved phase from Lake Chaohu were measured by (GC–MS). The composition and seasonal variation were investigated. The diffusive air–water exchange flux was estimated by a two-film model, and the uncertainty in the flux calculations and the sensitivity of the parameters were evaluated. The following results were obtained: (1) the average residual levels of all PAHs (PAH16) in the atmosphere from Lake Chaohu were 60.85 ± 46.17 ng m−3 in the gaseous phase and 14.32 ± 23.82 ng m−3 in the particulate phase. The dissolved PAH16 level was 173.46 ± 132.89 ng L−1. (2) The seasonal variation of average PAH16 contents ranged from 43.09 ± 33.20 ng m−3 (summer) to 137.47 ± 41.69 ng m−3 (winter) in gaseous phase, from 6.62 ± 2.72 ng m−3 (summer) to 56.13 ± 22.99 ng m−3 (winter) in particulate phase, and 142.68 ± 74.68 ng L−1 (winter) to 360.00 ± 176.60 ng L−1 (summer) in water samples. Obvious seasonal trends of PAH16 concentrations were found in the atmosphere and water. The values of PAH16 for both the atmosphere and the water were significantly correlated with temperature. (3) The monthly diffusive air–water exchange flux of total PAH16 ranged from −1.77 × 104 ng m−2 d−1 to 1.11 × 105 ng m−2 d−1, with an average value of 3.45 × 104 ng m−2 d−1. (4) The results of a Monte Carlo simulation showed that the monthly average PAH fluxes ranged from −3.4 × 103 ng m−2 d−1 to 1.6 × 104 ng m−2 d−1 throughout the year, and the uncertainties for individual PAHs were compared. (5) According to the sensitivity analysis, the concentrations of dissolved and gaseous phase PAHs were the two most important factors affecting the results of the flux calculations.  相似文献   

8.
The biogeochemical dynamics of 15 perfluorinated compounds (PFCs) were investigated in a heavily urbanised river (River Seine, Paris, France). The target compounds included C4-C10 sulfonates and C5-C14 acids; eleven PFCs were detected and ∑PFCs ranged between 31 and 91 ng L−1 (median: 47 ng L−1). The molecular pattern was dominated by the perfluoroalkyl sulfonates PFHxS and PFOS (>54% of ∑PFCs), which were the only PFCs quantified in both the dissolved and particulate phases. For these PFCs, the sorbed fraction positively correlated with suspended sediment levels. Total PFC levels negatively correlated with river flow rate, which varied between 150 and 640 m3 s−1. This suggests the predominance of point sources (likely WWTP effluent discharge), but a contribution of non-point sources such as combined sewer overflow could not be excluded. The annual PFC mass flow was estimated at 500 kg, which is less than observed for other large European rivers.  相似文献   

9.
Mt. Gongga area in southwest China was impacted by Hg emissions from industrial activities and coal combustion, and annual means of atmospheric TGM and PHg concentrations at a regional background station were 3.98 ng m−3 and 30.7 pg m−3, respectively. This work presents a mass balance study of Hg in an upland forest in this area. Atmospheric deposition was highly elevated in the study area, with the annual mean THg deposition flux of 92.5 μg m−2 yr−1. Total deposition was dominated by dry deposition (71.8%), and wet deposition accounted for the remaining 28.2%. Forest was a large pool of atmospheric Hg, and nearly 76% of the atmospheric input was stored in forest soil. Volatilization and stream outflow were identified as the two major pathways for THg losses from the forest, which yielded mean output fluxes of 14.0 and 8.6 μg m−2 yr−1, respectively.  相似文献   

10.
Organochlorine pesticides are persistent lipophilic organic pollutants and tend to accumulate in growing plants. During growth, cork is in contact with the open air for long periods (9-12 years). Owing to the previous widespread use of organochlorine pesticides and their high persistence in the environment, there is a risk that residues of such pesticides may be present in cork.In this study, the concentrations of 14 organochlorine pesticides—all of which are indicators of environmental pollution—were analyzed in cork bark samples from three regions in Spain and one in Portugal. In addition, the concentrations of 2,4,6-trichlorophenol (TCP) and 2,4,6-trichloroanisole (TCA) were also analyzed.Our results show only very low concentrations of lindane, γ-HCH (<2.6 ng g−1) and its byproducts α-HCH (<3.5 ng g−1) and β-HCH (<0.6 ng g−1).Among the DDT and its metabolites, only two were found: p,p′-DDT was found in a cork sample from Extremadura (0.1 ng g−1) and p,p′-DDE was present at a maximum concentration of 2.9 ng g−1 in a cork sample from Castile-La Mancha. However, all concentrations were well below the legal limit established by Regulation (EC) No. 396/2005 (10 ng g−1 in foodstuffs). We can conclude, therefore, that the cork samples we studied complied with food safety standards.  相似文献   

11.
Water extracts of atmospheric particulate matter (PM2.5) collected at the Storm Peak Laboratory (SPL) (3210 MSL, 40.45° N, 106.74° W) were analyzed for a wide variety of polar organic compounds. The unique geographical character of SPL allows for extended observations/sampling of the free tropospheric interface. Under variable meteorological conditions between January 9th and January14th 2007, the most abundant compounds were levoglucosan (9–72 ng m?3), palmitic acid (10–40 ng m?3) and succinic acid (18–27 ng m?3). Of 84 analytes included in the GC–MS method, over 50 individual water extractable polar organic compounds (POC) were present at concentrations greater than 0.1 ng m?3. During a snow event (Jan. 11th–13th), the concentrations of several presumed atmospheric transformation compounds (dicarboxylic acids) were reduced. Lower actinic flux, reduced transport distance, and ice crystal scavenging may explain this variability. Diurnal averages over the sampling period revealed a higher total concentration of water extractable POC at night, 211 ng m?3 (105–265 ng m?3), versus day, 160 ng m?3 (137–205 ng m?3), which suggests a more aged nighttime aerosol character. This may be due to the increased daytime convective mixing of local primary emissions from the Yampa Valley. XAD resin extracts revealed a gas-phase partitioning of several compounds, and analysis of cloud water collected at this site in 2002 revealed a similar compound abundance trend. Levoglucosan, a wood smoke tracer was generally found to be the most abundant compound in both aerosol and cloud water samples. Variations in meteorological parameters and local/regional transport analysis play an important interpretive role in understanding these results.  相似文献   

12.
Twenty-four congeners of polychlorinated biphenyls (PCBs) were measured in 83 air samples and 20 elastic sealants samples of apartments with PCB-containing sealants. In addition, PCBs were measured in 21 air samples from reference apartments located in an uncontaminated section of the same estate. The PCBtot levels in the air of the contaminated section were 168-3843 ng m−3 (mean: 1030 ng m−3), while the mean levels in the reference apartments were 6.03 ng m−3. The sum of the 24 measured PCB congeners in sealants from the contaminated section was 187-221 680 mg kg−1. Principal component analysis revealed four groups among the sealant samples with different congener compositions, only two of which were clearly similar to known PCB mixtures, while two were not. Significant correlations and intercorrelations were observed between the lower chlorinated congeners in air and sealant, e.g. for PCB 28air and 28seal (p = 0.04) and for PCB 28air and 52air, 52seal. However, no correlation was observed between the lower chlorinated congeners and the sums of PCB (∑PCB6 or ∑PCB24) or the higher chlorinated congeners. Analysis of air concentrations in relation to questionnaire data indicated that the indoor air levels could be reduced by increased cleaning and airing frequencies.  相似文献   

13.
Mercury pollution is caused by artisanal and small-scale gold mining (ASGM) operations along the Cikaniki River (West Java, Indonesia). The atmosphere is one of the primary media through which mercury can disperse. In this study, atmospheric mercury levels are estimated using the native epiphytic fern Asplenium nidus complex (A. nidus) as a biomonitor; these estimates shed light on the atmospheric dispersion of mercury released during mining.Samples were collected from 8 sites along the Cikaniki Basin during September-November, 2008 and September-November, 2009.The A. nidus fronds that were attached to tree trunks 1-3 m above the ground were collected and measured for total mercury concentration using cold vapor atomic absorption spectrometry (CVAAS) after acid-digestion. The atmospheric mercury was collected using porous gold collectors, and the concentrations were determined using double-amalgam CVAAS.The highest atmospheric mercury concentration, 1.8 × 103 ± 1.6 × 103 ng m−3, was observed at the mining hot spot, and the lowest concentration of mercury, 5.6 ± 2.0 ng m−3, was observed at the remote site from the Cikaniki River in 2009. The mercury concentrations in A. nidus were higher at the mining village (5.4 × 103 ± 1.6 × 103 ng g−1) than at the remote site (70 ± 30 ng g−1). The distribution of mercury in A. nidus was similar to that in the atmosphere; a significant correlation was observed between the mercury concentrations in the air and in A. nidus (r = 0.895, P < 0.001, n = 14). The mercury levels in the atmosphere can be estimated from the mercury concentration in A. nidus using a regression equation: log (HgA.nidu/ng g−1) = 0.740 log (HgAir/ng m−3) − 1.324.  相似文献   

14.

This work aimed to determine the seasonal variations of polycyclic aromatic hydrocarbons (PAHs) in airborne PM10 at two background sites (Masná—MS, Líšeň—LN) in Brno over a 5-year period (2009–2013). Samples were collected on quartz filters using a low-volume sampler by continual filtration. Concentrations of PAHs in collected PM10 samples were determined using a gas chromatography with a mass spectrometer as a detector. A different number of PAHs were determined to be at each site, i.e., 11 PAHs at the MS site and six PAHs at the LN site, and similarities between them were identified using non-parametric analysis of variance. Potential sources were identified using principal component analysis (PCA) and PAHs diagnostic ratios. The work also focused on health risk assessment. This was estimated using toxic equivalent factors to calculate individual lifetime cancer risk, which quantifies risk of exposure to PAHs for specific age groups. The average 11-PAH concentrations in M|S site annually ranged from 19.28 ± 19.02 ng m−3 (2011) to 40.37 ± 21.35 ng m−3 (2013). With regard to the LN site, the average six-PAH concentrations annually ranged from 3.64 ± 3.87 ng m−3 (2009) and 5.27 ± 6.19 ng m−3 (2012). PCA and diagnostic ratios indicate the main sources to be traffic emissions and coal combustion. Health risk assessment showed carcinogenic risk under limit value in all cases.

  相似文献   

15.
Ambient speciated mercury concentrations including total gaseous mercury (TGM), gaseous divalent mercury (Hg(II)), and particulate mercury (Hg(p)) were measured on the roof of the Graduate School of Public Health building in Seoul, Korea from February 2005 to February 2006. The average concentrations were 3.22 ± 2.10 ng m?3, 27.2 ± 19.3 pg m?3, and 23.9 ± 19.6 pg m?3 for TGM, Hg(II), and Hg(p), respectively. Hg(II) and Hg(p) concentrations were higher during the daytime than during the nighttime, probably because of high photochemical activity. Hg0 concentrations were not significantly correlated with ozone however a positive correlation between ozone and Hg(II) was found during periods of high humidity. Eighteen days were characterized as pollution events with 24 h average PM2.5 concentrations >65 μg m?3. The average concentrations of TGM and Hg(p) during these events were 1.4–2 times higher than those during non-pollution events. In order to identify the contribution of long-range transported mercury to the enhanced mercury concentrations in Korea, an episode was defined as a period with hourly average TGM and CO concentrations higher than the monthly average TGM and CO concentrations and with significant enhancement of both TGM and CO concentrations for at least 10 h. A total of 70 episodes were identified during the sampling period: 36 local episodes and 34 long-range transport episodes. The mean ΔTGM/ΔCO slope for all episodes was 0.0063 ng m?3 ppbv?1 which agreed well with the slope (0.0036–0.0074 ng m?3 ppbv?1) found in previous studies that identified long-range transport of TGM from China. The mean slope during non-events was 0.0011 ng m?3 ppbv?1. Back-trajectory analysis showed that during episodes, air parcels arrived mostly from the major industrial areas in China (n = 25, 73%), followed by Japan (n = 4, 12%), Yellow Sea (n = 3, 9%), and Russia (n = 2, 6%).  相似文献   

16.
Agricultural wastes are a source of steroid estrogens and, if present, conjugated estrogens may add to the estrogen load released to soil and aquatic environments. Dairy shed effluent samples were collected from 18 farms for analysis of steroid estrogens by GC-MS, conjugated estrogens by LC-MS-MS, and estrogenic activity by E-screen in vitro bioassay. 17α-estradiol was found at highest concentrations (median 730 ng l−1), followed by estrone (100 ng l−1) and 17β-estradiol (24 ng l−1). Conjugated estrogens (estrone-3-sulfate, 17α-estradiol-3-sulfate and 17β-estradiol-3,17-disulfate) were measured in most samples (12-320 ng l−1). Median estrogenic activity was 46 ng l−1 17β-estradiol equivalents. Conjugated estrogens contributed up to 22% of the total estrogen load from dairy farming, demonstrating their significance. Steroid estrogens dominated overall estrogenic activity measured in the samples. Significantly, 17α-estradiol contributed 25% of overall activity, despite potency 2% that of 17β-estradiol, highlighting the importance in environmental risk assessments of this previously neglected compound.  相似文献   

17.
Oxalate, the anion of oxalic acid, is one of the most abundant measurable organic species in atmospheric aerosols. Traditionally, this bifunctional species has been measured by gas chromatography (GC) after derivatization to butyl ester and by ion chromatography (IC) without derivatization. However, there are few published comparisons of the two techniques. Here, we report the results of an intercomparison study for the measurement of oxalic acid in Arctic aerosols (<2.5 μm, n = 82) collected in 1992 using GC and IC. The concentrations of oxalic acid by GC ranged from 6.5–59.1 ng m?3 (av. 26.0 ng m?3, median 26.2 ng m?3) whereas those by IC ranged from 6.6–52.1 ng m?3 (av. 26.6 ng m?3, median 25.4 ng m?3). They showed a good correlation (r = 0.84) with a slope of 0.96. Thus, observations of oxalate obtained by GC employing dibutyl esters are almost equal to those by IC. Because the accuracy of oxalic acid by GC method largely depends on the method used, it is important to strictly examine the recovery in each study.  相似文献   

18.
Sediments from a remote lake of northeastern Tibetan Plateau were analyzed for polycyclic aromatic hydrocarbons (PAHs) and trace metals. USEPA priority PAHs, ranged from 11 in 1860 to 279 ng g−1 in 2002, while, the deposition fluxes were in the range of 0.2-11.4 ng cm−2 yr−1. Similarly, from 1860 to 2002, an increased trend of Hg flux was observed (0.5-3.2 ng cm−2 yr−1). Remarkable increase of PAHs and Hg concentration began from 1970, nearly the same period of the “Reform and Open” Policy had been embarked (1978) in China. Good correlations were found between concentrations of Pb, Zn, Cd, As, Hg, and PAHs, which suggested the sources of these chemicals in the sediment is analogous, likely from anthroprogenic sources. Based on isomer ratios, PAHs in core were dominantly from the incomplete combustion of coal. Owing to the proximity to dust source area (Qaidam Basin) and the close association between PAHs, Hg, Pb, and particle matters, atmospheric dust-transport and deposition might be the main pathways that pollutants enter into Qinghai Lake.  相似文献   

19.
Yang G  Ma L  Xu D  Li J  He T  Liu L  Jia H  Zhang Y  Chen Y  Chai Z 《Chemosphere》2012,87(8):845-850
Arsenic levels and speciation in the total suspended particles (TSPs) were quantitatively determined by high performance liquid chromatography on-line coupled with hydride generation atomic fluorescence spectrometry in Beijing, China from February 2009 to March 2011. The high TSP levels fluctuated between 0.07 and 0.79 mg m−3, with a mean level of 0.32 ± 0.17 mg m−3. The total arsenic concentrations ranged from 0.03 to 0.31 μg m−3 (mean: 0.13 ± 0.06 μg m−3) in Beijing‘s air. The concentrations of As(III) and As(V) ranged from 0.73 to 20 ng m−3 (mean: 4.7 ± 3.6 ng m−3) and from 14 to 2.5 × 102 ng m−3 (mean: 67 ± 35 ng m−3), respectively. As levels and speciation demonstrated relative higher levels in spring and autumn and lower values in summer and winter. As(V) accounted for 81-99% of the extractable species in the TSP samples which showed that As(V) was the major fraction of the extractable As. Organoarsenic species, monomethylarsonate (MMA) and dimethylarsinate (DMA) were not found in all samples. Higher values of enrichment factors demonstrated that arsenic in TSP mainly come from anthropogenic sources. High As and its species levels in air and respiratory exposure (0.30-0.84 μg d−1) attributed to higher excess cancer risk ((4.2 ± 2.0) × 10−4) for people in Beijing.  相似文献   

20.
In streams, chemicals such as 17β-estradiol (E2) are likely to occur in pulses. We investigated uptake and biomarker responses in juvenile brown trout (Salmo trutta) of 3- or 6-h pulses of concentrations up to 370 ng E2 L−1. Uptake by the fish was estimated from disappearance of E2 from tank water. A single 6-h pulse of 370 ng E2 L−1 increased the plasma vitellogenin concentration, liver Erα- and vitellogenin-mRNA. Exposure to 150-160 ng E2 L−1 for 6 h increased vitellogenin in one experiment but not in another. Two 6-h pulses had a larger effect one pulse. Brown trout in the size range 24-74 g took up E2 linearly with time and exposure concentration with a concentration ratio rate of 20.2 h−1. In conclusion, the threshold for induction of estrogenic effects in juvenile brown trout at short term pulse exposure appears to be in the range 150-200 ng E2 L−1.  相似文献   

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