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1.
Multivariate statistical techniques were used to investigate source apportionment and source/sink relationships for polycyclic aromatic hydrocarbons (PAHs) in the urban and adjacent coastal atmosphere of Chicago/Lake Michigan in 1994–1995. The PAH signatures for the atmospheric particle phase, surface water particle phase and sediments indicate that atmospheric deposition is the major source of PAHs to the sediments and water column particulate phase of Lake Michigan. The PAH signature for the atmospheric gas phase and water dissolved phase indicate an intimate linkage between the lake and its overlying atmosphere. A modified factor analysis-multiple regression model was successfully applied to the source apportionment of atmospheric PAHs (gas+particle). Coal combustion accounted for 48±5% of the ΣPAH concentration in both the urban and adjacent coastal atmosphere, natural gas combustion accounted for 26±2%, coke ovens accounted for 14±3%, and vehicle emissions (gas+diesel) accounted for 9±4%. Each is an identified source category for the region. These results are consistent with the mix of fossil fuel combustion sources and ratios of indicator PAHs.  相似文献   

2.
Successions of lake ecosystems from clear-water, macrophyte-rich conditions into turbid states with abundant phytoplankton have taken place in many shallow lakes in China. However, little is know about the change of carbon fluxes in lakes during such processes. We conducted a case study in Lake Biandantang to investigate the change of carbon fluxes during such a regime shift. Dissolved aquatic carbon and gaseous carbon (methane (CH4) and carbon dioxide (CO2)) across air–water interface in three sites with different vegetation covers and compositions were studied and compared. CH4 emissions from three sites were 0.62±0.36, 0.70±0.36, and 1.31±0.57 mg m−2 h−1, respectively. Correlation analysis showed that macrophytes, rather than phytoplankton, directly positively affected CH4 emission. CO2 fluxes of three sites in Lake Biandantang were significantly different, and the average values were 77.8±20.4, 52.2±14.1 and 3.6±26.8 mg m−2 h−1, respectively. There were an evident trend that the larger macrophyte biomass, the lower CO2 emissions. Correlation analysis showed that in different sites, dominant plant controlled CO2 flux across air–water interface. In a year cycle, the percents of gaseous carbon release from lake accounting for net primary production were significantly different (from 39.3% to 2.8%), indicating that with the decline of macrophytes and regime shift, the lake will be a larger carbon source to the atmosphere.  相似文献   

3.
4.
Accidental releases of waste water from the first Czechoslovak nuclear power plant, A1, caused contamination of sediments of the Dudváh river, flowing into the Vah river, in Slovakia. Rather high concentrations of 137Cs and 90Sr (2150Bq dm−3 and 215Bq dm−3, respectively) were found in bottom sediments of a former channel of the re-engineered river body at a distance of about 250 m from a village, Siladice, with water-supply wells. In order to assess the possibility of contamination of the wells, underground migration of both radionuclides from the contaminated area was simulated using an original layered convection-diffusion model. Kd values determined in laboratory experiments were used. The analysis of the hydrological situation in the area reveals that the critical condition is a dominant horizontal groundwater flow near the water table in the direction from the Váh bank to Siladice, in the periods when the contaminated body lies under the water table. The simulation calculated under conservative conditions showed that the contamination of water-supply wells would not exceed permissible concentration limits.  相似文献   

5.
《Chemosphere》1996,32(11):2097-2113
The concentrations of pentachlorophenol (PCP), polychlorinated dibenzo-p-dioxins (PCDDs) polychlorinated dibensofurans (PCDFs) and organochlorine and organophosphorus pesticides in water, sediments and biota from the Lake Rotorua catchment were determined to evaluate the relative significance of various contaminants and their potential sources. PCP was found in water, sediments and biota (fish and freshwater mussels) and the highest concentrations in water (3.62 μ g.L−1) and in sediments (400 ng.g−1 dry weight (DW) were found in and near a stream that had been affected by PCP contamination from a sawmill. PCDD and PCDF concentrations in all cases, except for the waters and sediments of the stream near to the sawmill, were relatively low compared to values reported in the literature for similar sites. Negligible pesticide contamination was found in the Lake Rotorua catchment. Pesticides found included low concentrations of p.p′-DDE, p.p-TDE and dieldrin in rainbow trout from the lake.  相似文献   

6.
Dry atmospheric deposition contributes a significant amount of phosphorus to the Everglades of South Florida. Measurement of this deposition is problematic, because samples often are contaminated to varying degrees by bird droppings and other foreign materials. This study attempted to detect and remove the outliers in phosphorus (P) flux rates measured from dry deposition samples. Visual inspection of the samples, recorded in field notes, found that 30.1% of the samples contained animal droppings and frogs. Some of the samples with droppings and frogs (2.3%) had P values greater than 884 μg P m−2 d−1 (a value twice the standard deviation of the raw data mean), and were removed from further analysis. Outlier detection statistics based on a linear regression were then used for additional data screening. Eight stations in the network of 19 were removed because high contamination precluded the use of the regression model. Of the remaining samples, 15.7% were identified through the regression procedure as contaminated and were removed. The 11 station mean for P dry deposition was 85.8±79.0 μg P m−2 d−1, prior to the regression analysis, and 74.8±75.1 μg P m−2 d−1 after removal.  相似文献   

7.
The aim of this study is to present the organic and inorganic spectral aerosol module-radiative (ORISAM-RAD) module, allowing the 3D distribution of aerosol radiative properties (aerosol optical depth, single scattering albedo and asymmetry parameter) from the ORISAM module. In this work, we test ORISAM-RAD for one selected day (24th June) during the ESCOMPTE (expérience sur site pour contraindre les modèles de pollution atmosphérique et de transport d’emissions) experiment for an urban/industrial aerosol type. The particle radiative properties obtained from in situ and AERONET observations are used to validate our simulations. In a first time, simulations obtained from ORISAM-RAD indicate high aerosol optical depth (AOD)0.50–0.70±0.02 (at 440 nm) in the aerosol pollution plume, slightly lower (10–20%) than AERONET retrievals. In a second time, simulations of the single scattering albedo (ωo) have been found to well reproduce the high spatial heterogeneities observed over this domain. Concerning the asymmetry parameter (g), ORISAM-RAD simulations reveal quite uniform values over the whole ESCOMPTE domain, comprised between 0.61±0.01 and 0.65±0.01 (at 440 nm), in excellent agreement with ground based in situ measurements and AERONET retrievals. Finally, the outputs of ORISAM-RAD have been used in a radiative transfer model in order to simulate the diurnal direct radiative forcing at different locations (urban, industrial and rural). We show that anthropogenic aerosols strongly decrease surface solar radiation, with diurnal mean surface forcings comprised between −29.0±2.9 and −38.6±3.9 W m−2, depending on the sites. This decrease is due to the reflection of solar radiations back to space (−7.3±0.8<ΔFTOA<−12.3±1.2 W m−2) and to its absorption into the aerosol layer (21.1±2.1<ΔFATM<26.3±2.6 W m−2). These values are found to be consistent with those measured at local scale.  相似文献   

8.
Vehicle emissions can constitute a major share of ambient concentrations of many volatile organic compounds (VOCs) and other air pollutants in urban areas. Especially high concentrations may occur at curbsides, vehicle cabins, and other microenvironments. Such levels are not reflected by monitoring at fixed sites. This study reports on measurements of VOCs made from buses and cars in Detroit, MI. A total of 74 adsorbent tube samples were collected on 40 trips and analyzed by GC-MS for 77 target compounds. Three bus routes, selected to include residential, commercial and heavily industrialized areas, were sampled simultaneously on four sequential weeks during morning and afternoon rush hour periods. Nineteen compounds were regularly detected and quantified, the most prevalent of which included hexane/2-methyl pentane (15.6±5.8 μg m−3), toluene (10.2±7.9 μg m−3), m,p-xylene (6.8±4.7 μg m−3), benzene (4.5±3.0 μg m−3), 1,2,4-trimethylbenzene (4.0±2.6 μg m−3), o-xylene (2.2±1.6 μg m−3), and ethylbenzene (2.1±1.5 μg m−3). VOC levels in bus interiors and outdoor levels along the roadway were similar. Despite the presence of large industrial sources, route-to-route variation was small, but temporal variation was large and statistically significant. VOC compositions and trends indicate the dominance of vehicle sources over the many industrial sources in Detroit with the possible exceptions of styrene and several chlorinated VOCs. In-bus levels exceeded concentrations at fixed site monitors by a factor of 2–4. VOC concentrations in Detroit traffic are generally comparable to levels measured elsewhere in the US and Canada, but considerably lower than measured in Asia and Europe.  相似文献   

9.
《Chemosphere》1987,16(10-12)
The presence of polychlorinated biphenyls (PCBs) was investigated in samples of water, suspended particles, sediments and fish from the Kupa river, Croatia, Yugoslavia, along a river stretch extending up to 10 km upstream and 200 km downstream of the primary contaminated karst region. Contamination was due to improper disposal of industrial waste discharge. The PCB levels detected in the samples collected downstream ranged from 1 to 52 ng 1−1 for water, from 50 to 190 μg kg−1 for suspended particles and from 8 to 39 μg kg−1 for the sediment. A wide range of PCB concentrations, from 0.1 to 42.3 μg g−1, which were measured in edible portions of different fish confirmed a long-term contamination of the river with PCBs. As the Kupa may be classified among low to moderately contaminated waters, it is essential that the investigations of the presence and behaviour of PCBs in the river and its environment be continued.  相似文献   

10.
Diffusion coefficients (T=23±2 °C) and accessible porosities for HTO, 36Cl and 125I were measured on Opalinus Clay (OPA) samples from the Mont Terri Underground Rock Laboratory (URL) using the through-diffusion technique. The direction of transport (diffusion) was perpendicular to bedding. Special cells that allowed the application of confining pressure were designed and constructed. The pressures ranged from 1 to 5 MPa, the latter value simulating the overburden at the Mont Terri URL (about 200 m). The test solution used in the experiments was a synthetic version of the Opalinus Clay pore water, which has Na+ and Cl as the main components (I=0.42 M).The measured values of the effective diffusion coefficients (De) and rock capacity factors (α) are: De=1.2–1.5×10−11 m2 s−1 and α=0.09–0.11 for HTO, De=4.0–5.5×10−12 m2 s−1 and α=0.05 for 36Cl and De=3.2–4.6×10−12 m2 s−1 and α=0.07–0.10 for 125I. For non-sorbing tracers (HTO, 36Cl) the rock capacity factor α is equal to the diffusion-accessible porosity . The experimental results showed that pressure only had a small effect on the value of the diffusion coefficients. Increasing the pressure from 1 to 5 MPa resulted in a decrease of the diffusion coefficient of 17% for HTO, 28% for 36Cl and 30% for 125I. Moreover, the diffusion coefficients for 36Cl and 125I are smaller than for HTO, which is consistent with an effect arising from anion exclusion.The diffusion coefficients of HTO and 125I measured in this study are in good agreement with recent measurements at three other laboratories performed within the framework of a laboratory comparison exercise. The values of the diffusion-accessible porosities show a larger degree of scatter.  相似文献   

11.
A historical input of trace metals into tidal marshes fringing the river Scheldt may be a cause for concern. Nevertheless, the specific physicochemical form, rather than the total concentration, determines the ecotoxicological risk of metals in the soil. In this study the effect of tidal regime on the distribution of trace metals in different compartments of the soil was investigated. As, Cd, Cu and Zn concentrations in sediment, pore water and in roots were determined along a depth profile. Total sediment metal concentrations were similar at different sites, reflecting pollution history. Pore water metal concentrations were generally higher under less flooded conditions (mean is (2.32 ± 0.08) × 10−3 mg Cd L−1 and (1.53 ± 0.03) × 10−3 mg Cd L−1). Metal concentrations associated with roots (mean is 202.47 ± 2.83 mg Cd kg−1 and 69.39 ± 0.99 mg Cd kg−1) were up to 10 times higher than sediment (mean is 20.48 ± 0.19 mg Cd kg−1 and 20.42 ± 0.21 mg Cd kg−1) metal concentrations and higher under dryer conditions. Despite high metal concentrations associated with roots, the major part of the metals in the marsh soil is still associated with the sediment as the overall biomass of roots is small compared to the sediment.  相似文献   

12.
The atmospheric reaction of the methylthiyl radical (CH3S) with O3 was investigated as a function of temperature (259–381 K), in the pressure range of 25–300 Torr, using the technique of laser photolysis/laser-induced fluorescence. The resulting Arrhenius expression, with an uncertainty of ±2σ, was k1(T=259–381 K)=(1.02±0.30)×10−12 exp[(432±77) K/T] cm3 molecule−1 s−1. The obtained rate constant k1 was independent of pressure over the limited range employed. Our results are compared with the previous studies carried out, at single temperature and as a function of temperature, by different techniques.  相似文献   

13.
The quantum yield of the phototransformation of 4-nitrophenol has been evaluated as 4.5×10−5±0.6×10−5 at pH=2; at 3.0×10−5±0.6×10−5 at pH=5.5; 1.8×10−5±0.5×10−5 at pH=8.3. However the half-life is relatively low and no accumulation of aromatic or quinonic products was observed. Hydroquinone (QH2) is the main organic primary product formed when an air-saturated or degassed solution was irradiated in 365 nm monochromatic light (about 80% of the 4-nitrophenol initially converted at pH=5.5 in the absence of oxygen). In air-saturated neutral or acidic solution, the formation of NO3 ions accounted for about 80% of the 4-nitrophenol converted, but in degassed medium a mixture NO : NO2 : NO3 is formed. An heterolytical mechanism of photohydrolysis with primary formation of QH2 and HNO2 is suggested. Several by-products as benzoquinone, 4-nitrosophenol, 4-nitrocatechol and nitrohydroquinone are formed according to the conditions. Many secondary reactions are involved as the disproportionation or the oxidation of HNO2, the oxidation of QH2 by HNO2 and oxidations induced by excitation of NO2 and NO3.  相似文献   

14.
In the Ellen catchment on the Pinjarra Plain, NE of Perth in Western Australia, cadmium from fertilisers is starting to leach from soils. About 70% of surface soils in the Ellen catchment are sandy and often on top of a shallow ephemeral water table. Adsorption of Cd in the sandy soils of the Ellen catchment was studied by batch adsorption and by leaching small columns of soil. Adsorption of Cd increases linearly with increasing soil organic matter content and exponentially with increasing pH. Cadmium is significantly mobilised in the sandy soils by dissolved organic matter.The capacity of most of the sandy soils in the Ellen catchment to adsorb phosphate from fertiliser has been saturated. Resulting concentrations in Ellen Brook average 500 μg L−1 P. Cadmium is adsorbed more strongly in the sandy soils than phosphate and is just starting to leach into Ellen Brook. From a comparison of Cd/P ratios in water, soils and fertiliser, cadmium concentrations in Ellen Brook are estimated to be at 10–30% of their maximum for complete breakthrough from soils. Present concentrations of Cd in Ellen Brook average 0.1 μg L−1 and are estimated to approach the maximum for complete breakthrough in 100 yr. Maximum Cd concentrations in Ellen Brook could range from 0.6 to 2 μg L−1, depending on rates of input with fertiliser and future increases in agricultural land use in the catchment.Breakthrough curves, resulting from leaching Cd through small columns of sandy soil, indicate that adsorption significantly increases the effective hydrodynamic dispersion of Cd. Longitudinal dispersivities, measured at pore-water velocities of 0.7–14 m day−1, were 5 cm for Cd and 0.1–0.2 cm for chloride. The much greater dispersion of Cd in the sandy soils than of chloride is shown not to be caused by non-equilibrium adsorption.  相似文献   

15.
Long-term study of air pollution plays a decisive role in formulating and refining pollution control strategies. In this study, two 12-month measurements of PM2.5 mass and speciation were conducted in 00/01 and 04/05 to determine long-term trend and spatial variations of PM2.5 mass and chemical composition in Hong Kong. This study covered three sites with different land-use characteristics, namely roadside, urban, and rural environments. The highest annual average PM2.5 concentration was observed at the roadside site (58.0±2.0 μg m−3 (average±2σ) in 00/01 and 53.0±2.7 μg m−3 in 04/05), followed by the urban site (33.9±2.5 μg m−3 in 00/01 and 39.0±2.0 μg m−3 in 04/05), and the rural site (23.7±1.9 μg m−3 in 00/01 and 28.4±2.4 μg m−3 in 04/05). The lowest PM2.5 level measured at the rural site was still higher than the United States’ annual average National Ambient Air Quality Standard of 15 μg m−3. As expected, seasonal variations of PM2.5 mass concentration at the three sites were similar: higher in autumn/winter and lower in summer. Comparing PM2.5 data in 04/05 with those collected in 00/01, a reduction in PM2.5 mass concentration at the roadside (8.7%) but an increase at the urban (15%) and rural (20%) sites were observed. The reduction of PM2.5 at the roadside was attributed to the decrease of carbonaceous aerosols (organic carbon and elemental carbon) (>30%), indicating the effective control of motor vehicle emissions over the period. On the other hand, the sulfate concentration at the three sites was consistent regardless of different land-use characteristics in both studies. The lack of spatial variation of sulfate concentrations in PM2.5 implied its origin of regional contribution. Moreover, over 36% growth in sulfate concentration was found from 00/01 to 04/05, suggesting a significant increase in regional sulfate pollution over the years. More quantitative techniques such as receptor models and chemical transport models are required to assess the temporal variations of source contributions to ambient PM2.5 mass and chemical speciation in Hong Kong.  相似文献   

16.
A high-throughput screening method using selective pressurized liquid extraction (SPLE) and enzyme-linked immunosorbent assay (ELISA) for monitoring dioxins in sediment and soil is described. SPLE conditions were developed by extracting sediment or soil together with alumina, 10% AgNO3 in silica, and sulfuric acid impregnated silica (acid silica) using dichloromethane (DCM) as the solvent at 100 °C and 2000 psi. Post-extraction cleanups were not required for ELISA. Two reference sediments (National Institute of Standards and Technology SRM 1944 and Wellington Laboratories WMS01) were analyzed by the SPLE–ELISA method. The ELISA utilized a polyclonal antibody and 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) as the calibrant. Recoveries of ELISA-derived TCDD equivalents (EQ) relative to the expected gas chromatography/high resolution mass spectrometry (GC/HRMS) derived dioxin toxic equivalent (TEQ) values were 116 ± 11% for SRM 1944 and 102 ± 13% for WMS01. ELISA TCDD EQs were consistent with the dioxin TEQs as measured by GC/HRMS for 25 soil/sediment samples from seven different contaminated sites. The ELISA had an approximate method detection limit of 10 pg g−1 with a precision of 2.6–29% based on the relative percentage difference (%RPD) for duplicate samples. Estimated sample throughput for the SPLE–ELISA was three times or more than that of the GC/HRMS method employing PLE with a multi-column cleanup.  相似文献   

17.
Groundwater provides about 30% of water requirements in Ontario, but farm families depend almost entirely on private wells. Major potential contaminants on farms are nitrate (NO3), pathogenic microorganisms, pesticides and petroleum derivatives. A survey of farm drinking-water wells was conducted throughout the Province of Ontario, Canada, in 1991 and 1992 and tested for these contaminants. The main objectives of the survey were to determine the quality and safety of drinking water for farm families, and determine the effect of agricultural management on groundwater quality at a provincial scale. Four farm wells were chosen in each township where >50% of the land area was used for agricultural production. Elsewhere one well per township was usually sampled. Within each township the types of farming activity and dominant soils were additional criteria for selection. The network comprised 1292 of the estimated 500,000 water-wells in Ontario, and the study conformed to a stratified random survey. A subset of 160 wells, chosen by farm type, soil, and the presence or absence of a fuel storage tank, was investigated for the presence of petroleum derivatives: benzene, toluene, ethyl benzene, and xylene. About 40% of farm wells tested contained one or more of the target contaminants above the maximum acceptable concentration; 34% of wells had more than the maximum acceptable number of coliform bacteria, 14% contained NO3-N concentrations above 10 mg l−1 limit and about 7% were contaminated with both bacteria and NO3. Only six wells contained pesticide residues above the interim maximum acceptable concentration (IMAC), but pesticides were detected in 7% of wells in winter and in 11% in summer. No wells contained detectable petroleum derivatives. These results for NO3 contamination were not significantly different from those reported for a survey of Ontario wells for the period 1950–1954, but the frequency of contamination by Escherichia coli was greater in the present study. None of the point sources investigated contributed significantly to the NO3 contamination. The percentage of wells contaminated by coliform bacteria decreased significantly with increasing separation of the well from the feedlot or exercise yard on livestock farms. A full statistical model including the type of well construction, depth, age and soil hydrologic group was developed to describe the frequency of NO3 contamination.  相似文献   

18.
Chromium (Cr) is a well-known human carcinogen and a potential reproductive toxicant, but its contribution to ocean pollution is poorly understood. The aim of this study was to provide a global baseline for Cr as a marine pollutant using the sperm whale (Physeter macrocephalus) as an indicator species. Biopsies were collected from free-ranging whales around the globe during the voyage of the research vessel The Odyssey. Total Cr levels were measured in 361 sperm whales collected from 16 regions around the globe detectable levels ranged from 0.9 to 122.6 μg Cr g tissue−1 with a global mean of 8.8 ± 0.9 μg g−1. Two whales had undetectable levels. The highest levels were found in sperm whales sampled in the waters near the Islands of Kiribati in the Pacific (mean = 44.3 ± 14.4) and the Seychelles in the Indian Ocean (mean = 19.5 ± 5.4 μg g−1). The lowest mean levels were found in whales near the Canary Islands (mean = 3.7 ± 0.8 μg g−1) and off of the coast of Sri Lanka (mean = 3.3 ± 0.4 μg g−1). The global mean Cr level in whale skin was 28-times higher than mean Cr skin levels in humans without occupational exposure. The whale levels were more similar to levels only observed previously in human lung tissue from workers who died of Cr-induced lung cancer. We conclude that Cr pollution in the marine environment is significant and that further study is urgently needed.  相似文献   

19.
Hexabromocyclododecanes (HBCDs) are now emerging ubiquitous contaminants due to their wide usage, persistence and toxicities. To investigate the bioaccumulative characteristics of HBCDs, sediments, Winkle (Littorina littorea), crucian carp (Carassius carassius) and loach (Misgurnus anguillicaudatus) were collected from two streams near an E-waste dismantling site in China, and HBCD exposure test was then conducted on Chinese rare minnow. The concentration of HBCDs was 14 ng g−1 dry weight in sediments, 186, 377 and 1791 ng g−1 lipid weight in winkle, crucian carp and loach, respectively. γ-HBCD was found to be the dominant diastereoisomer in the sediments (63% of total HBCDs). However, α-HBCD was selectively accumulated in the biotic samples and contributed to 77%, 63% and 63% of total HBCDs in winkle, crucian carp and loach, respectively. Moreover, an enrichment of (−)-enantiomers of α- and γ-HBCD were found in the winkle. The reverse results were observed in the crucian carp and loach. Similar observations of diastereoisomeric and enantiomeric composition were obtained in Chinese rare minnow with those found in the crucian carp and loach. These results indicate that the freshwater species from the streams are contaminated by HBCDs. α-HBCD can be selectively accumulated in organisms and the accumulative characteristics are enantioselective among species.  相似文献   

20.
Amorphous ferric oxyhydroxide is being used to treat groundwater contaminated with uranium(VI); the compound also has potential for use as a component in in situ chemical barriers. To quantitatively evaluate its effectiveness in such applications, adsorption of uranium(VI) onto amorphous ferric oxyhydroxide was experimentally investigated under a wide range of uranium(VI) (8.40·10−7−2.10·10−3 mol L−1; 0.2–500 mg L−1), sulfur(VI) (0–0.07 mol L−1; 0–2240 mg L−1) and carbon(IV) (0–0.0195 mol L−1; 0–234 mg L−1) concentrations, and pH-values (4–9.6). The adsorption behavior of uranium(VI) (uranyl ion and its complexes) is similar to that of other cations; it exhibits a sharp rise in the extent of adsorption with increasing pH. Interactions among uranyl complexes and surface sites are interpreted using a site complexation model. Although the model does not incorporate electrostatics and includes only a single type of adsorption site, it provides a reasonable match to measured adsorption and proton exchange data. The simplicity of the model and the resulting reduction in computational demand allow its efficient incorporation into coupled reaction-transport models.  相似文献   

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