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1.
Changes in deposition of gaseous divalent mercury (Hg(II)) and particulate mercury (Hg(p)) in New Hampshire due to changes in local sources from 1996 to 2002 were assessed using the Industrial Source Complex Short Term (ISCST3) model (regional and global sources and Hg atmospheric reactions were not considered). Mercury (Hg) emissions in New Hampshire and adjacent areas decreased significantly (from 1540 to 880 kg yr−1) during this period, and the average annual modeled deposition of total Hg also declined from 17 to 7.0 μg m−2 yr−1 for the same period. In 2002, the maximum amount of Hg deposition was modeled to be in southern New Hampshire, while for 1996 the maximum deposition occurred farther north and east. The ISCST3 was also used to evaluate two future scenarios. The average percent difference in deposition across all cells was 5% for the 50% reduction scenario and 9% for the 90% reduction scenario.  相似文献   

2.
From October 2003 to September 2004, we conducted a detailed study on the mass balance of total mercury (THg) and methylmercury (MeHg) of Dongfeng (DF) and Wujiangdu (WJD) reservoirs, which were constructed in 1992 and 1979, respectively. Both reservoirs were net sinks for THg on an annual scale, absorbing 3319.5 g km−2 for DF Reservoir, and 489.2 g km−2 for WJD Reservoirs, respectively. However, both reservoirs were net sources of MeHg to the downstream ecosystems. DF Reservoir provided a source of 32.9 g MeHg km−2 yr−1, yielding 10.3% of the amount of MeHg that entered the reservoir, and WJD Reservoir provided 140.9 g MeHg km−2 yr−1, yielding 82.5% of MeHg inputs. Our results implied that water residence time is an important variable affecting Hg methylation rate in the reservoirs. Our study shows that building a series of reservoirs in line along a river changes the riverine system into a natural Hg methylation factory which markedly increases the %MeHg in the downstream reservoirs; in effect magnifying the MeHg buildup problem in reservoirs.  相似文献   

3.
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   

4.
Physical characterization and chemical analysis of settled dusts collected in Xi’an from November 2007 to December 2008 show that (1) dust deposition rates ranged from 14.6 to 350.4 g m−2 yr−1. The average deposition rate (76.7 g m−2 yr−1) ranks the 11th out of 56 dust deposition rates observed throughout the world. The coal-burning power was the major particle source; (2) on average (except site 4), ∼10% of the settled dusts having size <2.6, ∼30% having size <10.5, and >70% having size <30 μm; (3) the concentrations for 20 out of 27 elements analyzed were upto 18 times higher than their soil background values in China. With such high deposition rates of dusts that contain elevated levels of toxic elements, actions should be taken to reduce emission and studies are needed to assess the potential impacts of settled particles on surface ecosystem, water resource, and human health in the area.  相似文献   

5.
Long-term mercury dynamics in UK soils   总被引:1,自引:0,他引:1  
A model assuming first-order losses by evasion and leaching was used to evaluate Hg dynamics in UK soils since 1850. Temporal deposition patterns of Hg were constructed from literature information. Inverse modelling indicated that 30% of 898 rural sites receive Hg only from the global circulation, while in 51% of cases local deposition exceeds global. Average estimated deposition is 16 μg Hg m−2 a−1 to rural soils, 19 μg Hg m−2 a−1 to rural and non-rural soils combined. UK soils currently hold 2490 tonnes of reactive Hg, of which 2140 tonnes are due to anthropogenic deposition, mostly local in origin. Topsoil currently releases 5.1 tonnes of Hg0 per annum to the atmosphere, about 50% more than the anthropogenic flux. Sorptive retention of Hg in the lower soil exerts a strong control on surface water Hg concentrations. Following decreases in inputs, soil Hg concentrations are predicted to decline over hundreds of years.  相似文献   

6.
The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m−2 compared to an annual precipitation Hg flux of 8.7±0.5 μg m−2 (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m−2) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m−2). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m−2).  相似文献   

7.
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   

8.
Mercury (Hg) concentration profiles and historical accumulation rates were determined in three 210Pb-dated cores from a peat deposit in the vicinity of a lead (Pb) smelter at Příbram, Czech Republic. The Hg concentrations in peat samples ranged from 66 to 701 μg kg−1. Cumulative Hg inventories from each core (for the past 150 yr) varied by a factor of 1.4 (13.6–18.5 mg Hg m−2), indicating variations of net Hg accumulation rate within the peat deposit. Historical changes in vegetation cover (leading to variable interception by trees) are probably responsible for this variation in space and time. The uncorrected Hg accumulation rates peaked between the 1960s and 1980s (up to 226 μg m−2 yr−1). Recent findings show that Hg records from peat tend to overestimate historical levels of Hg deposition. Therefore we used the mass loss compensation factor (MLCF) to normalize Hg accumulation rates. These corrected Hg accumulation rates were significantly lower (maximum 129 μg m−2 yr−1) and better corresponded to changes in historical smelter emissions, which were highest in the 1960s. The agreement between the corrected Hg accumulation rates in the uppermost peat sections (2–38 μg m−2 yr−1) and biomonitoring of atmospheric deposition by mosses in several recent years (4.7–34.4 μg m−2 yr−1) shows the usefulness of MLCF application on Hg accumulation in peat archives. However, the MLCF correction was unsuitable for Pb. The recent Pb deposition rates obtained by an independent biomonitoring study using mosses (0.5–127 mg m−2 yr−1) were better correlated with net Pb accumulation rates recorded in peat (7–145 mg m−2 yr−1) than with corrected rates obtained by the MLCF approach (1–28 mg m−2 yr−1).  相似文献   

9.
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   

10.
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   

11.
Urban lakes are vulnerable to the accumulation of semivolatile organic compounds, such as PAHs from wet and dry atmospheric deposition. Little was reported on the seasonal patterns of atmospheric deposition of PAHs under Asian monsoon climate. Bulk (dry + wet) particle deposition, air-water diffusion exchange, and vapour wet deposition of PAHs in a small urban lake in Guangzhou were estimated based on a year-round monitoring. The total PAH particle deposition fluxes observed were 0.44-3.46 μg m−2 day−1. The mean air-water diffusive exchange flux was 20.7 μg m−2 day−1. The vapour deposition fluxes of PAHs ranged 0.15-8.26 μg m−2 day−1. Remarkable seasonal variations of particulate PAH deposition, air-water exchange fluxes and vapour wet deposition were influenced by seasonal changes in meteorological parameters. The deposition fluxes were predominantly controlled by the precipitation intensity in wet season whereas by atmospheric concentration in dry season.  相似文献   

12.
The main objective of this work was to assess the atmospheric concentrations and seasonal variations of selected POPs in a sub-alpine location where few data are available. A monitoring and research station was set up at the JRC Ispra EMEP site (Italy). We present and discuss a one-year data set (2005-2006) on PCB air concentrations. ∑7PCBs monthly averaged concentration varied from 31 to 76 pg m−3. Concentrations in the gas phase (21-72 pg m−3) were higher than those in the particulate phase (3-10 pg m−3). Advection of air masses and re-volatilization from local sources seem to play a dominant role as drivers of PCB atmospheric concentrations in the area. Indications of seasonal variation affecting PCB congener patterns and the gas/particulate partitioning were found. Modeling calculations suggest a predominant importance of the wet deposition in this region (1 μg m−2 yr−1 ∑7PCBs yearly total wet deposition flux; 650-2400 pg L−1 rainwater concentrations).  相似文献   

13.
Gaseous mercury fluxes from the forest floor of the Adirondacks   总被引:4,自引:0,他引:4  
The flux of gaseous elemental mercury (Hg0) from the forest floor of the Adirondack Mountains in New York (USA) was measured numerous times throughout 2005 and 2006 using a polycarbonate dynamic flux chamber (DFC). The Hg flux ranged between −2.5 and 27.2 ng m−2 h−1 and was positively correlated with temperature and solar radiation. The measured Hg emission flux was highest in spring, and summer, and lowest in winter. During leaf-off periods, the Hg emission flux was highly dependent on solar radiation and less dependent on temperature. During leaf-on periods, the Hg emission flux was fairly constant because the forest canopy was shading the forest floor. Two empirical models were developed to estimate yearly Hg0 emissions, one for the leaf-off period and one for the leaf-on period. Using the U.S. EPA's CASTNET meteorological data, the cumulative estimated emission flux was approx. 7.0 μg Hg0 m−2 year−1.  相似文献   

14.
A novel passive sampling technique using a funnel–adsorber–cartridge device was adopted and validated in the field during a long-term monitoring program on the atmospheric deposition of polycyclic aromatic hydrocarbons (PAHs) in three rural regions of southern Germany. Apart from seasonal variations, fairly stable annual deposition rates around 200 μg m−2 yr−1 for the sum of PAHs were obtained. The time-integrating passive samplers showed that spatial variability due to topography was negligible and differences between open-field and forest deposition were within a factor of 2. Based on correlations with ambient temperature, advection was identified as the most important factor that controls the atmospheric deposition of PAHs. Gas-adsorption contributes significantly to the deposition of the semivolatile compounds in forests, but particle deposition seems to be the major pathway for all PAHs.  相似文献   

15.

Due to its adverse impact on health, as well as its global distribution, long atmospheric lifetime and propensity for deposition in the aquatic environment and in living tissue, the US Environmental Protection Agency (US EPA) has classified mercury and its compounds as a severe air quality threat. Such widespread presence of mercury in the environment originates from both natural and anthropogenic sources. Global anthropogenic emission of mercury is evaluated at 2000 Mg year−1. According to the National Centre for Emissions Management (Pol. KOBiZE) report for 2014, Polish annual mercury emissions amount to approximately 10 Mg. Over 90% of mercury emissions in Poland originate from combustion of coal.

The purpose of this paper was to understand mercury behaviour during sub-bituminous coal and lignite combustion for flue gas purification in terms of reduction of emissions by active methods. The average mercury content in Polish sub-bituminous coal and lignite was 103.7 and 443.5 μg kg−1. The concentration of mercury in flue gases emitted into the atmosphere was 5.3 μg m−3 for sub-bituminous coal and 17.5 μg m−3 for lignite. The study analysed six low-cost sorbents with the average achieved efficiency of mercury removal from 30.6 to 92.9% for sub-bituminous coal and 22.8 to 80.3% for lignite combustion. Also, the effect of coke dust grain size was examined for mercury sorptive properties. The fine fraction of coke dust (CD) adsorbed within 243–277 μg Hg kg−1, while the largest fraction at only 95 μg Hg kg−1. The CD fraction < 0.063 mm removed almost 92% of mercury during coal combustion, so the concentration of mercury in flue gas decreased from 5.3 to 0.4 μg Hg m−3. The same fraction of CD had removed 93% of mercury from lignite flue gas by reducing the concentration of mercury in the flow from 17.6 to 1.2 μg Hg m−3. The publication also presents the impact of photochemical oxidation of mercury on the effectiveness of Hg vapour removal during combustion of lignite. After physical oxidation of Hg in the flue gas, its effectiveness has increased twofold.

  相似文献   

16.
Based on multi-year measurements of CH4 exchange in sub-daily resolution we show that clear-cutting of a forest in Southern Germany increased soil temperature and moisture and decreased CH4 uptake. CH4 uptake in the first year after clear-cutting (−4.5 ± 0.2 μg C m−2 h−1) was three times lower than during the pre-harvest period (−14.2 ± 1.3 μg C m−2 h−1). In contrast, selective cutting did not significantly reduce CH4 uptake. Annual mean uptake rates were −1.18 kg C ha−1 yr−1 (spruce control), −1.16 kg C ha−1 yr−1 (selective cut site) and −0.44 kg C ha−1 yr−1 (clear-cut site), respectively. Substantial seasonal and inter-annual variations in CH4 fluxes were observed as a result of significant variability of weather conditions, demonstrating the need for long-term measurements. Our findings imply that a stepwise selective cutting instead of clear-cutting may contribute to mitigating global warming by maintaining a high CH4 uptake capacity of the soil.  相似文献   

17.
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   

18.
This paper reports mercury (Hg) concentrations and fluxes in precipitation that was collected from 2006 to 2008 at three sites in Canada: sub-Arctic boreal forest, sub-Arctic coast, and southern Alberta, using cold-adapted precipitation collectors which operated reliably at temperatures below ?30 °C during the study. The southern Alberta site (Crossfield) may be influenced by Calgary urban air, whereas the sub-Arctic coastal (Churchill, Manitoba) and boreal forest (Fort Vermilion, Alberta) sites are in more remote northern areas. Annual mean Hg concentrations in precipitation (5.0–9.2 ng L?1) at the study sites were in the lower half of the range reported for southern Canada and the USA by the Mercury Deposition Network (MDN). But owing to typically low precipitation rates, gross wet Hg fluxes (0.54–2.0 μg m?2 yr?1) were among the lowest reported by MDN, with Crossfield having about twice the flux in 2007 of the other two sites. Flux was significantly correlated with precipitation, and thus was highest in summer (June–August) and lowest during winter, a pattern typical of other temperate continental locations. There was no evidence of higher wet Hg fluxes or concentrations in springtime at Churchill where atmospheric mercury depletion events (AMDEs) occur. Measured gross deposition fluxes at the study locations were ~2–8 times lower than estimated by GEOS-Chem and GRAHM atmospheric models. The largest discrepancy occurred for Churchill, which raises the question of how well Hg deposition from AMDEs is described by current models. Better agreement between measurements and models was obtained from MDN stations in Alberta and Alaska, where wet Hg fluxes were 2–10 times higher than the study sites either because of power plant emissions (Alberta), or because of high precipitation rates (Alaska).  相似文献   

19.
《Chemosphere》2007,66(11):2477-2484
Atmospheric Hg transfer to the forest soil through litterfall was investigated in a primary rainforest at Ilha Grande (Southeast Brazil) from January to December 1997. Litter mass deposition reached 10.0 t ha−1 y−1, with leaves composing 50–84% of the total litter mass. Concentrations of Hg in the total fallen litter varied from 20 to 244 ng g−1, with higher concentrations during the dry season, between June and August (225 ± 17 ng g−1), and lower concentrations during the rainy season (99 ± 54 ng g−1). This seasonal variability was reflected in the Hg flux through litterfall, which corresponded to a Hg input to the forest floor of 122 μg m−2 y−1, with average Hg deposition of 16.5 ± 1.5 μg m−2 month−1 during and just after the dry season (June–September) and 7.0 ± 3.6 μg m−2 month−1 in the rest of the year. The variability in meteorological conditions (determining atmospheric Hg availability to foliar scavenging) may explain the pulsed pattern of Hg deposition, since litterfall temporal variability was generally unrelated with such deposition, except by a peak in litterfall production in September. Comparisons with regional data on Hg atmospheric deposition show that litterfall promotes Hg deposition at Ilha Grande two to three orders of magnitude higher than open rainfall deposition in non-industrialized areas and approximately two times higher than open rainfall deposition in industrialized areas in Rio de Janeiro State. The observed input suggests that atmospheric Hg transfer through litterfall may explain a larger fraction of the total Hg input to forest soils in Southeast Brazil than those recorded at higher latitudes.  相似文献   

20.
The median total mercury concentration in 898 UK rural topsoils, sampled between 1998 and 2008, was 0.095 μg g−1. Approximate adjustment for unreactive metal produced an estimate of 0.052 μg g−1 for reactive Hg. The highest concentrations were in the north and west, where organic-rich soils with low bulk densities dominate, but the spatial pattern was quite different if soil Hg pools (mg m−2) were considered, the highest values being near to the industrial north of England and London. Possible toxic effects of Hg were best evaluated by comparison with soil Critical Limits expressed as ratios of Hg to soil organic matter, or soil solution Hg2+ concentrations, estimated by chemical speciation modelling. Only a few percent of the rural UK soils showed exceedance, and this also applied to rural soils from the whole of Europe. UK urban and industrial soils had higher Hg concentrations and more cases of exceedance.  相似文献   

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