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1.
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   

2.
Mercury wet deposition is dependent on both the scavenging of divalent reactive gaseous mercury (RGM) and atmospheric particulate mercury (Hg(p)) by precipitation. Estimating the contribution of precipitation scavenging of RGM and Hg(p) is important for better understanding the causes of the regional and seasonal variations in mercury wet deposition. In this study, the contribution of Hg(p) scavenging was estimated on the basis of the scavenging ratios of other trace elements (i.e., Cd, Cu, Mn, Ni, Pb and V) existing entirely in particulate form. Their wet deposition fluxes and concentrations in air, which were measured concurrently from April 2004 to March 2005 at 10 sites in Japan, were used in this estimation. The monthly wet deposition flux of mercury at each site correlated with the amount of monthly precipitation, whereas the Hg(p) concentrations in air tended to decrease during summer. There was a significant correlation (P<0.001) among the calculated monthly average scavenging ratios of trace elements, and the values in each month at each site were similar. Therefore, it is assumed the monthly scavenging ratio of Hg(p) is equivalent to the mean value of other trace elements. Using this scavenging ratio (W), the wet deposition flux (F) due to Hg(p) scavenging in each month was calculated by F=WKP, where K and P are the Hg(p) concentration and amount of precipitation, respectively. Relatively large fluxes due to Hg(p) scavenging were observed at a highly industrial site and at sites on the Japan Sea coast, which are strongly affected by the local sources and the long-range transport from the Asian continent, respectively. However, on average, at the 10 sites, the contribution of Hg(p) scavenging to the annual mercury deposition flux was 26%, suggesting that mercury wet deposition in Japan is dominated by RGM scavenging. This RGM should originate mainly from the in situ oxidation of Hg0 in the atmosphere.  相似文献   

3.
Due to high availability of adsorption sites, forested catchments could be net sinks for pollutant arsenic both during the period of increasing and decreasing pollution. We tested this hypothesis along a north-south pollution gradient in spruce die-back affected areas of Central Europe. For two water years (2007-2008), we monitored As fluxes via spruce-canopy throughfall, open-area precipitation, and runoff in four headwater catchments (Czech Republic). Since 1980, atmospheric As inputs decreased 26 times in the north, and 13 times in the south. Arsenic export by runoff was similar to atmospheric inputs at three sites, resulting in a near-zero As mass balance. One site exhibited a net export of As (2.2 g ha−1 yr−1). In contrast, the preceding period (1995-2006) showed much higher As fluxes, and higher As export. Czech catchments do not serve as net sinks of atmospheric As. A considerable proportion of old industrial arsenic is flushed out of the soil.  相似文献   

4.
Mean annual (1994-1996) budgets for Cd, Cu, Ni, Pb and Zn at two background, forested catchments, VK and HJ, in Finland are presented. Budgets for plots (VK3, HJ1 and HJ4) included throughfall (TF), litterfall (LF) and soil leaching fluxes, and for catchments terrestrial retention and leaching and lake sedimentation fluxes. Total deposition (TD) loads were relatively low (Cd < 0.1, Cu < 2, Ni < 1, Pb < 3 and Zn < 5 mg m-2 year-1) and that even in these areas almost half of the TD was in the form of dry deposition. Retention of TD within catchments was > or = 77% for all metals, except for Ni at VK (54%). For Cu and Pb, the retention was 94-97%. Most of the retention (74-97%) took place in the terrestrial part of the catchment, lake sedimentation accounting for the remainder. Plot-scale soil leaching fluxes at 40 cm of Cd, Cu (VK3) and Ni (VK3) were greater (> or = 100%) than TD inputs. Most of the catchment retention must therefore have taken place either deeper in the soil or in the lowland peatland areas. The humus layer was particularly effective in retaining Cu and Cd (65-81% and 51-78% of total inputs to the forest floor (TF + LF)). The retention of Pb by the humus layer was less than expected (26-54% of TF + LF). Litterfall was a particularly important internal flux for Zn.  相似文献   

5.
Environmental pollution by mercury (Hg) is a considerable environmental problem world-wide. Due to the occurrence of Hg volatilization from their soils, floodplains can function as an important source of volatile Hg. Soil temperature and soil water content related to flood dynamics are considered as important factors affecting seasonal dynamics of total gaseous mercury (TGM) fluxes. We quantified seasonal variations of TGM fluxes and conducted a laboratory microcosm experiment to assess the effect of temperature and moisture on TGM fluxes in heavily polluted floodplain soils. Observed TGM emissions ranged from 10 to 850 ng m−2 h−1 and extremely exceeded the emissions of non-polluted sites. TGM emissions increased exponentially with raised air and soil temperatures in both field (R2: 0.49-0.70) and laboratory (R2: 0.99) experiments. Wet soil material showed higher TGM fluxes, whereas the role of soil water content was affected by sampling time during the microcosm experiments.  相似文献   

6.
Total mercury (TotHg) and methyl mercury (MeHg) concentrations were studied in runoff from eight small (0.02-1.3 km2) boreal forest catchments (mineral soil and peatland) during 1990-1995. Runoff waters were extremely humic (TOC 7-70 mg l-1). TotHg concentrations varied between 0.84 and 24 ng l-1 and MeHg between 0.03 and 3.8 ng l-1. TotHg fluxes from catchments ranged from 0.92 to 1.8 g km-2 a-1, and MeHg fluxes from 0.03 to 0.33 g km-2 a-1. TotHg concentrations and output fluxes measured in runoff water from small forest catchments in Finland were comparable with those measured in other boreal regions. By contrast, MeHg concentrations were generally higher. Estimates for MeHg output fluxes in this study were comparable at sites with forests and wetlands in Sweden and North America, but clearly higher than those measured at upland or agricultural sites in other studies. Peatland catchments released more MeHg than pure mineral soil or mineral soil catchments with minor area of peatland.  相似文献   

7.
I X Tsiros 《Chemosphere》2001,44(2):99-107
Dynamics of airborne mercury deposited onto catchment areas is investigated within the framework of a simulation model. Model results show that, for a particular atmospheric deposition rate, significant interannual variability in mercury transport flux in catchments is caused by climatology and corresponding differences in catchment soil loss rates; in comparison to the normal year, runoff flux increased by a factor of 2-3 for the wet year (rainfall 35% above normal) while for the dry year (rainfall 18% below normal) runoff flux decreased by factors of 5-7. The interaction of parameters describing soil type, topography and vegetation cover causes variability in both transport and emission fluxes among catchments; as soil loss rate increases by a factor of 5 due to variations in these parameters among the examined catchments, annual average transport flux increases by a factor of 3; and annual average emission flux of mercury (as Hg0) from soil to the atmosphere decreases by a factor of 2 due to the decreased levels of soil mercury associated with catchment soil loss increases. Seasonal variability of transport flux is associated with seasonal changes in precipitation and soil loss rates while seasonal changes of emission flux are primarily due to changes in soil moisture regime and temperature. Although modeled results are consistent with observational data from previous studies, they must be interpreted in a relative sense due to the screening-level character of this study.  相似文献   

8.
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   

9.
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   

10.
This work summarizes the results of a study of atmospheric wet and dry deposition fluxes of Deisopropyl-atrazine (DEA), Desethyl-atrazine (DET), Atrazine, Terbuthylazine, Alachlor, Metolachlor, Diflufenican, Fenoxaprop-p-ethyl, Iprodione, Isoproturon and Cymoxanil pesticides conducted in Strasbourg, France, from August 2000 through August 2001. The primary objective of this work was to calculate the total atmospheric pesticide deposition fluxes induced by atmospheric particles. To do this, a modified one-dimensional cloud water deposition model was used. All precipitation and deposition samples were collected at an urban forested park environment setting away from any direct point pesticide sources. The obtained deposition fluxes induced by atmospheric particles over a forested area showed that the dry deposition flux strongly contributes to the total deposition flux. The dry particle deposition fluxes are shown to contribute from 4% (DET) to 60% (cymoxanil) to the total deposition flux (wet + dry).  相似文献   

11.
Mercury (Hg) mining is an important anthropogenic source of atmospheric Hg emissions. The Guizhou Province in Southwestern China is a region with extensive artisanal mercury mining (AMM), but little Hg emission data from this area is available. Using a mass balance method, we estimated emission factors from artisanal mercury mining in Wuchuan mercury mining area (WMMA) and Gouxi area (GX). Average emission factors were 18.2% in WMMA (ranging from 6.9% to 32.1%) and 9.8% in GX (ranging from 6.6% to 14.5%), respectively, which were 2.2–36.4 times higher than the literature values used to estimate Hg emission from Hg mining. Furthermore, the average Hg emission factor of AMM in WMMA was much higher than that in GX, indicating that double condensation processes practiced in GX resulted in higher recoveries and lower emission factors compared to single condensation process applied in WMMA. Atmospheric Hg emission was estimated to be 3.7–9.6 metric tons in 2004 for WMMA and 1.3–2.7 metric tons in 2006 for GX, indicating artisanal Hg mining was an important atmospheric Hg emission source in the study area.  相似文献   

12.
Total gaseous mercury (Hg) fluxes from large (7.3×5.5×4.5 m, L×W×D) climate-controlled gas exchange mesocosms (Ecologically Controlled Enclosed Lysimeter Laboratories or EcoCELLs) containing tallgrass prairie soil–plant monoliths were measured from 2002 to 2005. EcoCELL Hg fluxes (calculated based on the difference in air Hg concentrations inside mesocosms and in incoming air, soil area of the monoliths, and airflow through the system) indicated a net annual emission of 102 μg m−2, while soil Hg fluxes measured simultaneously using a dynamic flux chamber were an order of magnitude lower. Since Hg fluxes measured from empty EcoCELLs in winter and when housing the soil–plant monoliths at the same time of year were similar, we hypothesized that the Hg signal generated by the tallgrass prairie soil–plant monoliths was too low to be detected using the EcoCELL technology. Because mesocosm Hg exchange was correlated with solar radiation and temperature, with the largest emissions occurring at midday and in the summer, we also hypothesized that the flux from mesocosm infrastructure would change over time. Limited by the ongoing experiment, the EcoCELLs were manipulated to test the above hypotheses. When monoliths were completely covered and excluded from the exchange with the surrounding air, mesocosm Hg exchange was unaffected. Furthermore, removal of vegetation at the end of each growing season did not affect mesocosm Hg fluxes. Tests with changing mesocosm airflow also indicated that the signal from the tallgrass prairie monoliths was not being measured. These results suggest that, although EcoCELLs performed well in a study using Hg contaminated soils and have been successfully applied to understand processes controlling Hg fluxes, there are limitations of this technology for quantifying Hg exchange from background substrates. Prior to the use of similar systems the detection limit and Hg exchange from an empty system need to be carefully quantified.  相似文献   

13.
Atmospheric deposition of phthalate esters in a subtropical city   总被引:1,自引:0,他引:1  
In Chinese cities, air pollution has become a serious and aggravating environmental problem undermining the sustainability of urban ecosystems and the quality of urban life. Bulk atmospheric deposition samples were collected two-weekly, from February 2007 to January 2008, at three representative areas, one suburban and two urbanized, in the subtropical city, Guangzhou, China, to assess the deposition fluxes and seasonal variations of phthalate esters (PAEs). Sixteen PAE congeners in bulk deposition samples were measured and the depositional fluxes of ∑16PAEs ranged from 3.41 to 190 μg m?2 day?1, and were highly affected by local anthropogenic activities. The significant relationship between PAEs and particulate depositional fluxes (correlation coefficient R2 = 0.72, P < 0.001) showed PAEs are associated primarily with particles. Temporal flux variations of PAEs were influenced by seasonal changes in meteorological parameters, and the deposition fluxes of PAEs were obviously higher in wet season than in dry season. Diisobutyl phthalate (DiBP), Di-n-butyl phthalate (DnBP), and Di(2-ethylhexyl) phthalate (DEHP) dominated the PAE pattern in bulk depositions, which is consistent with a high consumption of the plasticizer market in China. PAE profiles in bulk deposition showed similarities exhibited in both time and space, and a weak increase of high molecular weight PAE (HMW PAE) contribution in the wet season compared to those in the dry season. Average atmospheric deposition fluxes of PAEs in the present study were significantly higher than those from other studies, reflecting strong anthropogenic inputs as a consequence of rapid industrial and urban development in the region.  相似文献   

14.
To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m−3), average Hg emission flux (162–27827 ng m−2 h−1) and average Hg dry deposition flux (0–9434 ng m−2 h−1) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.  相似文献   

15.
One question in the use of plants as biomonitors for atmospheric mercury (Hg) is to confirm the linear relationships of Hg concentrations between air and leaves. To explore the origin of Hg in the vegetable and grass leaves, open top chambers (OTCs) experiment was conducted to study the relationships of Hg concentrations between air and leaves of lettuce (Lactuca sativa L.), radish (Raphanus sativus L.), alfalfa (Medicago sativa L.) and ryegrass (Lolium perenne L.). The influence of Hg in soil on Hg accumulation in leaves was studied simultaneously by soil Hg-enriched experiment. Hg concentrations in grass and vegetable leaves and roots were measured in both experiments. Results from OTCs experiment showed that Hg concentrations in leaves of the four species were significantly positively correlated with those in air during the growth time (p?<?0.05), while results from soil Hg-enriched experiment indicated that soil-borne Hg had significant influence on Hg accumulation in the roots of each plant (p?<?0.05), and some influence on vegetable leaves (p?<?0.05), but no significant influence on Hg accumulation in grass leaves (p?>?0.05). Thus, Hg in grass leaves is mainly originated from the atmosphere, and grass leaves are more suitable as potential biomonitors for atmospheric Hg pollution. The effect detection limits (EDLs) for the leaves of alfalfa and ryegrass were 15.1 and 22.2 ng g–1, respectively, and the biological detection limit (BDL) for alfalfa and ryegrass was 3.4 ng m–3.  相似文献   

16.
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m?2 h?1), emission in the summer (2.5 ng m?2 h?1), near zero flux in the fall (0.3 ng m?2 h?1), and emission in the winter (4.1 ng m?2 h?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.  相似文献   

17.
The effects of various factors including turbidity, pH, DOC, temperature, and solar radiation on the concentrations of total mercury (TM) and dissolved gaseous mercury (DGM) were investigated in an artificial reservoir in Korea. Episodic total mercury accumulation events occurred during the rainy season as turbidity increased, indicating that the TM concentration was not controlled by direct atmospheric deposition. The DGM concentration in surface water ranged from 3.6 to 160 pg/L, having a maximum in summer and minimum in winter. While in most previous studies DGM was controlled primarily by a photo-reduction process, DGM concentrations tracked the amount of solar radiation only in winter when the water temperature was fairly low in this study. During the other seasons microbial transformation seemed to play an important role in reducing Hg(II) to Hg(0). DGM increased as dissolved organic carbon (DOC) concentration increased (p-value < 0.01) while it increased with a decrease of pH (p-value < 0.01).  相似文献   

18.
Land use has obvious influence on surface water quality; thus, it is important to understand the effects of land use patterns on surface water quality. This study explored the relationships between land use patterns and stream nutrient levels, including ammonium-N (NH4 +-N), nitrate-N (NO3 ?-N), total N (TN), dissolved P (DP), and total P (TP) concentrations, in one forest and 12 agricultural catchments in subtropical central China. The results indicated that the TN concentrations ranged between 0.90 and 6.50 mg L?1 and the TP concentrations ranged between 0.08 and 0.53 mg L?1, showing that moderate nutrient pollution occurred in the catchments. The proportional areal coverages of forests, paddy fields, tea fields, residential areas, and water had distinct effects on stream nutrient levels. Except for the forest, all studied land use types had a potential to increase stream nutrient levels in the catchments. The land use pattern indices at the landscape level were significantly correlated to N nutrients but rarely correlated to P nutrients in stream water, whereas the influence of the land use pattern indices at the class level on stream water quality differentiated among the land use types and nutrient species. Multiple regression analysis suggested that land use pattern indices at the class level, including patch density (PD), largest patch index (LPI), mean shape index (SHMN), and mean Euclidian nearest neighbor distance (ENNMN), played an intrinsic role in influencing stream nutrient quality, and these four indices explained 35.08 % of the variability of stream nutrient levels in the catchments (p<0.001). Therefore, this research provides useful ideas and insights for land use planners and managers interested in controlling stream nutrient pollution in subtropical central China.  相似文献   

19.
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   

20.
Using the well-known Regional Atmospheric Modelling System (RAMS) version 4.3 an integrated system able to simulate the atmospheric mercury cycle has been developed. Basic processes of the mercury atmospheric cycle have been incorporated into the atmospheric model. The model deals with elemental Hg (Hg0), divalent gaseous Hg (Hg2) and particulate Hg (HgP). Wet deposition mechanisms used to describe the removal of Hg2 and HgP are merged with the detailed cloud microphysical scheme in order to provide better representation of the wet deposition processes. The advantages of this approach have been examined through results intercomparison with simulated Hg wet deposition using CMAQ-Hg from previous work for two evaluation periods: 4 April–2 May 1995, and 20 June–18 July 1995. An attempt to clarify the main parameters that affect wet deposition mechanism of mercury is also made.  相似文献   

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