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1.
Environmental properties of organic matter contained halogen and sulfur were studied in sediments of bleached kraft pulp mill effluent (BKME) recipient lakes and 2 m3 outdoor enclosures (mesocosms). The BKME contributed to 1% (v/v) of the total water flow in the lake downstream of the pulp mill where the sediments contained 1.7 to 4 mg of tetrahydrofuran extractable organic halogen (EOX-Cl) and 0.6 to 0.8 mg of tetrahydrofuran extractable organic sulfur (EOS-S) g−1 of organic matter. Upstream sediment contained 0.03 mg of EOXCl and 0.7 mg of EOS-S g−1 of organic matter. EOX was a better indicator for the influence of BKME in the recipient sediment than EOS. The polarity of BKME contained EOX corresponded to log Kow of < 1, and that of the downstream sediment contained EOX to > 4.5. HP-SEC analysis of the molecular weight distribution (MWD) of the EOX showed a peak between 300 to 600 g mol−1 for the BKME and between 1000 to 2000 g mol−1 for the downstream sediment. The MWD of the BKME contained EOS peaked at 300 to 1000 g mol−1, and that of the downstream sediment contained EOS at 1000 to 5000 g mol−1. These results indicate that BKME contained organic halogen and sulfur undergo major structural transformations when incorporated into sediment. The biota-to-sediment accumulation factor (BSAF) of EOX from sediments formed downstream of the mill and in the mesocosms to the lipids ofLumbriculus variegatus was 0.4 to 0.7. This is of a similar order of magnitude to the BSAF reported for 2,3,7,8-tetrachlorodibenzop-dioxin and 2,3,7,8-tetrachlorodibenzofuran.  相似文献   

2.
Atmospheric lead (Pb) pollution during the last century in central Yunnan province, one of the largest non-ferrous metal production centers in China, was reconstructed using sediment cores collected from Fuxian and Qingshui Lakes. Lead concentrations and isotopic ratios (207Pb/206Pb and 208Pb/206Pb) were measured in sediment cores from both lakes. The operationally defined chemical fractions of Pb in sediment core from Fuxian Lake were determined by the optimized BCR procedure. The chronology of the cores was reconstructed using 210Pb and 137Cs dating methods. Similar three-phase variations in isotopic ratios and enrichment factors of Pb were observed in the sediment cores from both lakes. Before the 1950s, the sediment data showed low 207Pb/206Pb and 208Pb/206Pb ratios and enrichment factors (EFs?=?~1), indicating that the sedimentary Pb was predominantly of lithogenic origin. However, these indices were increased gradually between the 1950s and the mid-1980s, implying an atmospheric Pb deposition. The EFs and isotopic ratios of Pb reached their peak during recent years, indicating aggravating atmospheric Pb pollution. The average anthropogenic Pb fluxes since the mid-1980s were estimated to be 0.032 and 0.053 g m?2 year?1 recorded in Fuxian and Qingshui cores, respectively. The anthropogenic Pb was primarily concentrated in the reducible fraction. Combining the results of Pb isotopic compositions and chemical speciations in the sediment cores and in potential sources, we deduced that recent aggravating atmospheric Pb pollution in central Yunnan province should primarily be attributed to regional emissions from non-ferrous metal production industries.  相似文献   

3.
The occurrence of halogenated organic compounds measured as a sum parameter and the evidence of chlorinated benzoic acids in four carbonaceous meteorites (Cold Bokkeveld, Murray, Murchison and Orgueil) from four independent fall events is reported. After AOX (Adsorbable organic halogen) and EOX (Extractable organic halogen) screening to quantify organically bound halogens, chlorinated organic compounds were analyzed by gas chromatography. AOX concentrations varying from 124 to 209 microg Cl/g d.w. were observed in carbonaceous meteorites. Ion chromatographic analysis of the distribution of organically bound halogens performed on the Cold Bokkeveld meteorite revealed that chlorinated and brominated organic compounds were extractable, up to 70%, whereas only trace amounts of organofluorines could be extracted. Chlorinated benzoic acids have been identified in carbonaceous meteorite extracts. Their presence and concentrations raise the question concerning the origin of halogenated, especially chlorinated, organic compounds in primitive planetary matter.  相似文献   

4.
Pine pollen concentrations in air at a semi-remote site in northern Wisconsin attained levels of 18 and 25 μ m−3 in late May and early June of 1979 and 1981, respectively. The upper and lower limits for the deposition velocity of pine pollen at this site are approximately 30 and 1.3 cm s−1, respectively. Consequently, the average annual pine pollen flux at this location for 1979 and 1981 was between 8.0 and 0.35 g m−2. Deposition of total phosphorus and organic C by pollen dispersal are about 5–100% and 11–240%, respectively, of the measured bulk atmospheric loading rate in the region. Pine pollen fluxes of water-extractable K are about 10–230% of the average annual wet deposition, while the fluxes of waterextractable NO3 and SO4−2 by pollen appear to be negligible in comparison to the total atmospheric deposition (wet plus dry deposition) by other particles. The annual pine pollen flux to Crystal Lake, an oligotrophic seepage lake in the region, was estimated to be 6.5 g m−2 during 1981. The deposition of total P by pollen to this lake was 5.8 kg a−1, which is 45 % of the external input of total phosphorus. About 60% of the total P in samples of Pinus strobus and P. resinosa was dissolved reactive P, which is readily available for plant uptake. Because P is the limiting nutrient for many lacustrine systems and pine pollen dispersal coincides with the period of phytoplankton blooms in temperate-region lakes, this episodic input of P may represent an important source for seepage lakes whose external inputs are dominated by atmospheric deposition.  相似文献   

5.
Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by 210Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m?2 yr?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m?2 yr?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m?2 yr?1 for preindustrial and 11.7 μg m?2 yr?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m?2 yr?1, which are lower than the modern sediment-based estimate of 11.7 μg m?2 yr?1, perhaps owing to inputs of dry-deposited Hg to the lakes.  相似文献   

6.
Lake-sediment records across the Northern Hemisphere show increases in atmospheric deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous studies have examined remote lakes affected by the global atmospheric Hg reservoir. In this study, we present Hg flux records from lakes in an urban/suburban setting of central New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a watershed that corresponds with the lake area. Sediment accumulation rates and dates were established by 210Pb. The pre-anthropogenic regional atmospheric Hg flux was estimated to be 3.0 μg m−2 yr−1 from Glacial Lake, which receives exclusively direct atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition.  相似文献   

7.
The main objectives of this study were to (a) study the interaction between N and P cycles in mining-affected aquatic systems and (b) to quantify release rates of sedimentary soluble reactive phosphorus (SRP) that may be related to this interaction. Sediment cores and water from Lake Bruträsket (Boliden, northern Sweden) were collected and a time series of water sampling and flow measurements was conducted in the Brubäcken stream connected to the lake. Factors affecting SRP release were studied in a sediment incubation experiment and water column experiments. Field and laboratory measurements indicated that pH and dissolved oxygen are two important factors for SRP release. At the end of the low-oxygen incubation, an SRP concentration of 56 μg?L?1 resulted in a sedimentary flux of 1.1 mg SRP?m?2?day?1. This is ~10 times higher than the flux of 0.12 mg SRP?m?2?day?1 obtained from depth integration of vertical SRP profiles measured in the lake, and ~100 times higher than the external flux of 0.014 mg SRP?m?2?d?1 into the lake (based on catchment area). Field measurements indicated that oxidation of organic matter and mining-related chemicals (ammonium and thiosulphates) may result in increased internal SRP flux from the sediment. Increased P loading in the lake as a result of low-oxygen conditions could change water column total nitrogen/total phosphorus ratios from 27 to 17, consequently changing the lake from being P-limited to be co-limited by N and P. The obtained findings point to possible interaction between the cycles of nitrogen (oxygen consumption) and P (flux from sediment) that may be important for nutrient regulation in mine water recipients.  相似文献   

8.
Surface sediment from large and eutrophic Lake Chaohu was investigated to determine the occurrence, spatial distribution, sources, and risks of polychlorinated biphenyls (PCBs) and heavy metals in one of the five biggest freshwater lakes in China. Total concentration of PCBs (Σ34PCBs) in Lake Chaohu was 672 pg g?1 dry weight (dw), with a range of 7 to 3999 pg g?1 dw, which was lower than other water bodies worldwide. The majority of heavy metals were detected at all sampling locations, except for Sr, B, and In. Concentrations of Al, Fe, Ca, Mn, Sr, Co, Zn, Cd, Pb, and Hg were similar to that reported for other lakes globally. Concentrations of K, Mg, Na, Li, Ga, and Ag were greater than the average, whereas those of Cr, Ni, and Cu were lower. Cluster analysis (CA) and positive matrix factorization (PMF) yielded accordant results for the source apportionment of PCBs. The technical PCBs and microbial degradation accounted for 34.2 % and 65.8 % of total PCBs using PMF, and PMF revealed that natural and anthropogenic sources of heavy metals accounted for 38.1 % and 61.8 %, respectively. CA indicated that some toxic heavy metals (e.g., Cd, In, Tl, and Hg) were associated with Ca–Na–Mg minerals rather than Fe–Mn minerals. The uncorrelated results between organic matter revealed by pyrolysis technology and heavy metals might be caused by the existence of competitive adsorption between organic matter and minerals. PCBs and heavy metals were coupling discharge without organochlorine pesticides (OCPs), but with polycyclic aromatic hydrocarbons (PAHs) and polybrominated diphenyl ethers (PBDEs). No sediment sample exceeded the toxic threshold for dioxin-like PCBs (dl-PCBs) set at 20 pg toxicity equivalency quantity (TEQ)?g?1, (max dl-PCBs, 10.9 pg TEQ g?1). However, concentrations of Ag, Cd, and Hg were at levels of environmental concern. The sediment in the drinking water source area (DWSA) was threatened by heavy metals from other areas, and some fundamental solutions were proposed to protect the DWSA.  相似文献   

9.
Intensive agricultural land use imposes multiple pressures on streams. More specifically, the loading of streams with nutrient-enriched soil from surrounding crop fields may deteriorate the sediment quality. The current study aimed to find out whether stream restoration may be an effective tool to improve the sediment quality of agricultural headwater streams. We compared nine stream reaches representing different morphological types (forested meandering reaches vs. deforested channelized reaches) regarding sediment structure, sedimentary nutrient and organic matter concentrations, and benthic microbial respiration. Main differences among reach types were found in grain sizes. Meandering reaches featured larger mean grain sizes (50–70 μm) and a thicker oxygenated surface layer (8 cm) than channelized reaches (40 μm, 5 cm). Total phosphorous amounted for up to 1,500 μg?g?1 DW at retentive channelized reaches and 850–1,050 μg?g?1 DW at the others. While N-NH4 accumulated in the sediments (60–180 μg?g?1 DW), N-NO3 concentrations were generally low (2–5 μg?g?1 DW). Benthic respiration was high at all sites (10–20 g O2 m?2?day?1). Our study shows that both hydromorphology and bank vegetation may influence the sediment quality of agricultural streams, though effects are often small and spatially restricted. To increase the efficiency of stream restoration in agricultural landscapes, nutrient and sediment delivery to stream channels need to be minimized by mitigating soil erosion in the catchment.  相似文献   

10.
During the summertime of 2007/2008, carbon dioxide (CO2) and methane (CH4) fluxes across air–water interface were investigated in the littoral zones of Lake Mochou and Lake Tuanjie, east Antarctica, using a static chamber technique. The mean fluxes of CO2 and CH4 were ?70.8 mgCO2 m?2 h?1 and 144.6 μgCH4 m?2 h?1, respectively, in the littoral zone of Lake Mochou; The mean fluxes were ?36.9 mgCO2 m?2 h?1 and 109.8 μgCH4 m?2 h?1, respectively, in the littoral zone of Lake Tuanjie. Their fluxes showed large temporal and spatial dynamics. The CO2 fluxes showed a significantly negative correlation with daily total radiation (DTR) and a weakly negative correlation with air temperature and water temperature, indicating that sunlight intensity controlled the magnitude of CO2 fluxes from the open lakes. The CH4 fluxes significantly correlated with local air temperature, water table and total dissolved solids (TDS), indicating that they were the predominant factors influencing CH4 fluxes. Summertime CO2 budgets in the littoral zones of Lake Mochou and Lake Tuanjie were estimated to be ?152.9 gCO2 m?2 and ?79.7 gCO2 m?2, respectively, and net CH4 emissions were estimated to be 312.3 mgCH4 m?2 and 237.2 mgCH4 m?2, respectively. Our results show that shallow, open, alga-rich lakes might be strong summertime CO2 absorbers and small CH4 emitters during the open water in coastal Antarctica.  相似文献   

11.
The dry deposition of atmospheric particulate matter can be a significant source of phosphorus (P) to oligotrophic aquatic ecosystems, including high-elevation lakes. In this study, measurements of the mass concentration and size distribution of aerosol particles and associated particulate P are reported for the southern Sierra Nevada, California, for the period July–October, 2008. Coarse and fine particle samples were collected with Stacked Filter Units and analyzed for Total P (TP) and inorganic P (IP) using a digestion-extraction procedure, with organic P (OP) calculated by difference. Particle size-resolved mass and TP distributions were determined concurrently using a MOUDI cascade impactor. Aerosol mass concentrations were significantly elevated at the study site, primarily due to transport from offsite and emissions from local and regional wildfires. Atmospheric TP concentrations ranged from 11 to 75 ng m?3 (mean = 37 ± 16 ng m?3), and were typically dominated by IP. Phosphorus was concentrated in the coarse (>1 μm diameter) particle fraction and was particularly enriched in the 1.0–3.2 μm size range, which accounted for 30–60% of the atmospheric TP load. Wildfire emissions varied widely in P content, and may be related to fire intensity. The estimated dry depositional flux of TP for each daily sampling period ranged between 7 and 118 μg m?2 d?1, with a mean value of 40 ± 27 μg m?2 d?1. Relative rates of dry deposition of N and P in the Sierra Nevada are consistent with increasing incidence of N limitation of phytoplankton growth and previously observed long-term eutrophication of lakes.  相似文献   

12.
Activity concentrations, inventories and activity ratios of 137Cs, 238Pu, 239?+?240Pu and 241Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m2 for 137Cs, 238Pu, 239?+?240Pu and 241Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The 238Pu/239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The 238Pu/239?+?240Pu and 239?+?240Pu/137Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.  相似文献   

13.

Acid deposition causes carbonate dissolution in watersheds and leads to profound impacts on water chemistry of lakes. Here, we presented a detailed study on the seasonal, spatial, and vertical variations of calcium and magnesium species in the overlying water, interstitial water, and sediment profiles in eutrophic Taihu Lake under the circumstance of regional acid deposition. The result showed that both the acid deposition and biomineralization in Taihu Lake had effects on Ca and Mg species. In the lake water, calcium carbonate was saturated or over-saturated based on long-term statistical calculation of the saturation index (SI). On the sediment profiles, significant difference in Ca and Mg species existed between the surface sediment (0–10 cm) and deeper sediments (>10 cm). The interstitial water Ca2+ and Mg2+, ion-exchangeable Ca and Mg in the surface sediment were higher than those in the deeper sediment. In the spring, when the acid deposition is more intensive, the acid-extracted Ca and Mg in the surface sediment were lower than that in the deeper sediment in the northwest lake, due to carbonate dissolution caused by the regional acid deposition. Spatially, the higher concentration of acid-extracted Ca and Mg in the northwest surface sediment than that in the east lake was observed, indicating the pronounced carbonate biomineralization by algae bloom in the northwest lake. Statistical analysis showed that acid deposition exerted a stronger impact on the variation of acid-extracted Ca and Mg in the surface sediment than the biomineralization in Taihu Lake. For the total Ca and Mg concentration in the spring, however, no significant change between the surface and deeper sediment in the northwest lake was observed, indicating that the carbonate precipitation via biomineralization and the carbonate dissolution due to acidic deposition were in a dynamic balance. These features are of major importance for the understanding of combined effects of acid deposition and eutrophication on freshwater lakes.

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14.
This report demonstrates that organic matter was an important factor in lake sediment 210Pbex dating. Sediment cores from lakes in central and western China with different-trophic levels were collected, and the 210Pbex activity and total organic carbon (TOC) were measured. The Rock-Eval pyrolysis technique was used to deconvolute TOC into free hydrocarbons (S1), thermally less-stable macromolecular organic matter (S2a), kerogen (S2b), and residual carbon (RC). The results show significant correlations between TOC and 210Pbex, particularly between S2a and 210Pbex, in all the sediment cores. This indicated that the algal-derived organic component S2a may play the most important role in controlling the distribution of 210Pbex. Scavenging by algal-derived organic matter may be the main mechanism. As chronology is the key to the understanding of pollution reconstruction and early diagenesis in sediments, more attention should be paid to the influence of organic matter on 210Pbex.  相似文献   

15.
Dissolved organic carbon (DOC) was measured in 483 precipitation samples collected at 10 sites in Northern China from December 2007 to November 2008. The annual volume-weighted mean (VWM) concentrations and wet deposition fluxes of DOC for 10 sites ranged from 2.4 to 3.9 mg C/L and 1.4 to 2.7 g C m?2 yr?1, respectively. The proportion of DOC to total organic carbon (TOC) was 79% on average, suggesting that a significant fraction of TOC was present as insoluble particulate organic carbon. Due to intensive domestic coal use for house heating and smaller dilution of scavenged organic carbon, higher VWM concentrations of DOC were observed during winter and spring than during summer and autumn. When precipitation events were classified via air mass back-trajectories, the mixed trajectories from SE and NW always corresponded to significantly higher DOC than those from SE or NW alone, coinciding with the centre of a low pressure system moved eastward and the wind direction changed from southeast to northwest. The results also showed that each site had a similar seasonal variation for DOC wet deposition flux. The largest flux occurred during the rainy season, and the lowest flux appeared during winter months. The product of the TC/DOC ratio and the DOC flux yielded an average TC wet deposition flux of 3.2 g C m?2 yr?1 in Northern China, accounting for 8.6% and 22% of the carbon sink magnitude (37 g C m?2 yr?1) in terrestrial ecosystems and anthropogenic carbon emissions (14 g C m?2 yr?1), respectively. This indicates that atmospheric wet deposition of TC is a significant carbon flux that cannot be neglected in regional models of the carbon cycle, and should be considered along with dry deposition in the removal mechanism for carbon from regional atmosphere.  相似文献   

16.
Abstract

Glyphosate, which is commercially available as Roundup®, was the widely used herbicide in Sri Lanka until 2015 and is suspected to be one of the causal factors for Chronic Kidney Disease of unknown etiology (CKDu). This research, therefore, aims at studying the presence of glyphosate and Aminomethylphosphonic acid (AMPA) in different environmental matrices in CKDu prevalent areas. Topsoil samples from agricultural fields, water samples from nearby shallow wells and lakes, and sediment samples from lakes were collected and analyzed for glyphosate and AMPA using the LC/MS. Glyphosate (270–690 µg/kg) and AMPA (2–8 µg/kg) were detected in all soil samples. Amorphous iron oxides and organic matter content of topsoil showed a strong and a moderate positive linear relationship with glyphosate. The glyphosate and inorganic phosphate levels in topsoil had a strong negative significant linear relationship. Presence of high valence cations such as Fe3+ and Al3+ in topsoil resulted in the formation of glyphosate-metal complexes, thus strong retention of glyphosate in soil. Lower levels of AMPA than the corresponding glyphosate levels in topsoil could be attributed to factors such as the strong adsorption capacity of glyphosate to soil and higher LOQ in the quantification of AMPA. The glyphosate levels of lakes were between 28 to 45 µg/L; no AMPA was detected. While trace levels of glyphosate (1–4 µg/L) were detected in all groundwater samples, AMPA (2–11µg/L) was detected only in four out of nine samples. Glyphosate was detected in all sediment samples (85–1000 µg/kg), and a strong linear relationship with the organic matter content was observed. AMPA was detected (1–15 µg/kg) in seven out of nine sediment samples. It could be inferred that the impact on CKDu by the levels of glyphosate and AMPA detected in the study area is marginal when compared with the MCL of the USEPA (700 µg/L).  相似文献   

17.
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   

18.

From simultaneous air and water polychlorinated biphenyl (PCB) measurements collected in September 2010, we re-evaluated the direction and magnitude of net air-water exchange of PCBs in southwest Lake Michigan and compared them with estimations made using similar approaches 15 years prior. Air and water samples were collected during a research expedition on Lake Michigan at 5 km off the coast of Chicago, with prevailing winds from the southwest of our location. Gas-phase ΣPCB concentrations ranged from 190 to 1100 pg m?3 with a median of 770 pg m?3, which is similar to the concentrations measured in the City of Chicago at the same time and similar to concentrations measured in this part of the lake over the last 20 years. Water dissolved-phase ΣPCB concentrations ranged from 150 to 170 pg L?1 with a median of 160 pg L?1, which is one-tenth of that measured in the 1990s. ?PCB net fluxes showed a slightly absorptive behavior, with a median of (?) 21 ng m?2 day?1 and an interquartile range of (?) 47 to (+) 5 ng m?2 day?1, where (?) and (+) fluxes indicate absorption and volatilization, respectively. Airborne PCB concentrations were higher when the winds were coming from Chicago and drive the deposition. Our fluxes are not significantly different from estimations from 1994 and 1995 and suggest that absorption of PCBs into the waters is slightly more prevalent than 15 years ago. It was confirmed that Chicago remains an important atmospheric source of PCBs to Lake Michigan.

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19.
Aerosol samples (TSP and PM10) during each season were collected at a national monitoring point in Shanghai in 2008. Halogens (Br, I) were determined in samples along with sodium (Na) by ICP-MS and ICP-OES after microwave digestion. In this report we focused on the concentration characteristics of halogen elements Br and I and their seasonal distributions. The mean annual concentrations of total Br and I were 24 ng m?3 and 12 ng m?3 for TSP, 21 ng m?3 and 9 ng m?3 for PM10, respectively. Concentrations of Br and I in TSP and PM10 were lowest in summer but an increase occurred in autumn and winter. Water-soluble Br and I accounted for about 32% of the total Br and I in aerosols, and about 68% of Br and I was non soluble which may be non-soluble organic species. These non-soluble organic species are present in aerosols in the possible binding forms as mineral dust, natural organic matter, and adsorption to black carbon or mineral material such as iron oxides. Soluble Br and I in PM10 extracted by a dilute acid solution (HNO3 + H2SO4) increased by 22% and 18%, respectively, compared with water-soluble Br and I. A positive correlation with Na and sea water enrichment factors for Br and I indicated that bromine and iodine in aerosols originated mostly from marine sources in Shanghai.  相似文献   

20.
Soil organic matter (SOM) releasing with dissolved organic matter (DOM) formed in solution was confirmed in a sediment/water system, and the effects of SOM releasing on the sorption of phenanthrene on sediments were investigated. Inorganic salt (0–0.1 mol L?1 NaCl) was used to adjust SOM releasing, and two sediments were prepared, the raw sediment (S1) from Weihe River, Shann’xi, China, and the eluted sediments with and without DOM supernatant remained, termed as S2a and S2b, respectively. The FTIR and 1H NMR analysis indicate that the low molecular weight hydrophilic SOM fraction released prior to the high molecular weight hydrophobic fraction. As a response, phenanthrene sorption kinetics on S1 showed atypical and expressed as three stages: rapid sorption, pseudo sorption with partial desorption, and slow sorption, thus a defined “sorption valley” occurred in kinetic curve. In all cases, partition dominates the sorption, and sorption capacity (Kd) ranked as S2b > S1 > S2a. Compared with the alterations of sediment characters, DOM solubilization produced by SOM releasing exhibited a greater inhibitory effect on sorption with a relative contribution of 0.67. Distribution coefficients (Kdoc) of PHE into DOM clusters were 2.10?×?104–4.18?×?104 L kg?1, however a threshold concentration of 6.83 mg L?1 existed in DOM solubilization. The study results will help to clarify PAHs transport and their biological fate in a sediment/water system.  相似文献   

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