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1.
Mercury air/surface exchange was measured over litter-covered soils with low Hg concentrations within various types of forests along the eastern seaboard of the USA. The fieldwork was conducted at six forested sites in state parks in South Carolina, North Carolina, New Jersey, Pennsylvania, New York and Maine from mid-May to early June 2005. The study showed that the Hg air/surface exchange was consistently very low and similar (overall daytime mean flux = 0.2 ± 0.9 ng m−2 h−1, n = 310, for all six sites monitored) with the various forest types. These flux values are comparable with those found in a year-long study in Tennessee (yearly daytime mean = 0.4 ± 0.5 ng m−2 h−1), but lower than many previous flux results reported for background soils. The Hg fluxes at all sites oscillated around zero, with many episodes of deposition (negative fluxes) occurring in both daytime and nighttime. While there were particular days showing significant correlations among the Hg air/surface exchange and certain environmental parameters, perhaps because of the low fluxes encountered, few significant correlations were found for any particular day of sampling between the Hg flux and environmental parameters such as solar radiation, soil temperature, air temperature (little variability seen), relative humidity, and ambient air Hg concentrations. Factors driving the Hg exchange as previously found for enriched soils may not hold for these background litter-covered forest soils. The results suggest that spatial variations of the Hg air/surface exchange were small among these different forest types for this particular time of year.  相似文献   

2.
This study focused on the development of a seasonal data set of the Hg air/surface exchange over soils associated with low Hg containing surfaces in a deciduous forest in the southern USA. Data were collected every month for 11 months in 2004 within Standing Stone State Forest in Tennessee using the dynamic flux chamber method. Mercury air/surface exchange associated with the litter covered forest floor was very low with the annual mean daytime flux being 0.4 ± 0.5 ng m−2 h−1 (n = 301). The daytime Hg air/surface exchange over the year oscillated between emission (81% of samples with positive flux) and deposition (19% of samples with negative flux). A seasonal trend of lower emission in the spring and summer (closed canopy) relative to the fall and winter (open canopy) was observed. Correlations were found between the air/surface exchange and certain environmental factors on specific days sampled but not collectively over the entire year. The very low magnitude of Hg air/surface exchange as observed in this study suggests that an improved methodology for determining and reporting emission fluxes is needed when the values of fluxes and chamber blanks are both very low and comparable. This study raises questions and points to a need for more research regarding how to scale the Hg air/surface exchange for surfaces with very low emissions.  相似文献   

3.
Gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) were measured over 2-week seasonal field campaigns near Salmon Falls Creek Reservoir in south-central Idaho from the summer of 2005 through the fall of 2006 and over the entire summer of 2006 using automated Tekran Hg analyzers. GEM, RGM, and particulate Hg (HgP) were also measured at a secondary site 90 km to the west in southwestern Idaho during the summer of 2006. The study was performed to characterize Hg air concentrations in the southern Idaho area for the first time, estimate Hg dry deposition rates, and investigate the source of observed elevated concentrations. High seasonal variability was observed with the highest GEM (1.91 ± 0.9 ng m−3) and RGM (8.1 ± 5.6 pg m−3) concentrations occurring in the summer and lower values in the winter (1.32 ± 0.3 ng m−3, 3.2 ± 2.9 pg m−3 for GEM, RGM, respectively). The summer-average HgP concentrations were generally below detection limit (0.6 ± 1 pg m−3). Seasonally averaged deposition velocities calculated using a resistance model were 0.034 ± 0.032, 0.043 ± 0.040, 0.00084 ± 0.0017 and 0.00036 ± 0.0011 cm s−1 for GEM (spring, summer, fall and winter, respectively) and 0.50 ± 0.39, 0.40 ± 0.31, 0.51 ± 0.43 and 0.76 ± 0.57 cm s−1 for RGM. The total annual RGM + GEM dry deposition estimate was calculated to be 11.9 ± 3.3 μg m−2, or about 2/3 of the total (wet + dry) deposition estimate for the area. Periodic elevated short-term GEM (2.2–12 ng m−3) and RGM (50–150 pg m−3) events were observed primarily during the warm seasons. Back-trajectory modeling and PSCF analysis indicate predominant source directions to the SE (western Utah, northeastern Nevada) and SW (north-central Nevada) with fewer inputs from the NW (southeastern Oregon and southwestern Idaho).  相似文献   

4.
Atmospheric mercury (Hg) is delivered to ecosystems via rain, snow, cloud/fog, and dry deposition. The importance of snow, especially snow that has passed through the forest canopy (throughfall), in delivering Hg to terrestrial ecosystems has received little attention in the literature. The snowpack is a dynamic system that links atmospheric deposition and ecosystem cycling through deposition and emission of deposited Hg. To examine the magnitude of Hg delivery via snowfall, and to illuminate processes affecting Hg flux to catchments during winter (cold season), Hg in snow in no-canopy areas and under forest canopies measured with four collection methods were compared: (1) Hg in wet precipitation as measured by the Mercury Deposition Network (MDN) for the site in Acadia National Park, Maine, USA, (2) event throughfall (collected after snowfall cessation for accumulations of >8 cm), (3) season-long throughfall collected using the same apparatus for event sampling but deployed for the entire cold season, and (4) snowpack sampling. Estimates (mean ± SE) of Hg deposition using these methods during the 91-day cold season in 2004–2005 at conifer sites showed that season-long throughfall Hg flux (1.80 μg/m2) < snowpack Hg (2.38 ± 0.68 μg/m2) < event throughfall flux (5.63 ± 0.38 μg/m2). Mercury deposition at the MDN site (0.91 μg/m2) was similar to that measured at other no-canopy sites in the area using the other methods, but was 3.4 times less than was measured under conifer canopies using the event sampling regime. This indicates that snow accumulated under the forest canopy received Hg from the overstory or exhibited less re-emission of Hg deposited in snow relative to open areas. The soil surface of field-scale plots were sprayed with a natural rain water sample that contained an Hg tracer (202Hg) just prior to the first snowfall to explore whether some snowpack Hg might be explained from soil emissions. The appearance of the 202Hg tracer in the snowpack (0–64% of the total Hg mass in the snowpack) suggests that movement of Hg from the soil into the snowpack is possible. However, as with any tracer study the 202Hg tracer may not precisely represent the reactivity and mobility of natural Hg in soils.  相似文献   

5.
The role of the major biogeochemical processes in Hg cycling at the sediment–water interface was investigated in the Grado Lagoon (Northern Adriatic Sea). This wetland system has been extensively contaminated from the Idrija Hg Mine (Slovenia) through the Isonzo River suspended load carried by tidal fluxes. Three approaches were used to study the sediment–water exchange of total Hg (THg), methylmercury (MeHg), reactive Hg (RHg) and dissolved gaseous Hg (DGHg): (1) estimation of diffusive fluxes from porewater and overlying water concentrations, (2) measurements of benthic fluxes using a deployed light benthic chamber in situ and (3) measurements of benthic fluxes during oxic–anoxic transition with a laboratory incubation experiment. The THg solid phase, ranging between 9.5 and 14.4 μg g−1, showed slight variability with depth and time. Conversely, MeHg contents were highest (up to 21.9 ng g−1) at the surface; they tended to decrease to nearly zero concentration with depth, thus suggesting that MeHg production and accumulation occur predominantly just below the sediment–water interface. Porewater MeHg concentrations (0.9–7.9 ng L−1, 0.15–15% of THg) varied seasonally; higher contents were observed in the warmer period. The MeHg diffusive fluxes (up to 17 ng m−2 day−1) were similar to those in the nearby Gulf of Trieste [Covelli, S., Horvat, M., Faganeli, J., Brambati, A., 1999. Porewater distribution and benthic flux of mercury and methylmercury in the Gulf of Trieste (Northern Adriatic Sea). Estuar. Coast. Shelf Sci. 48, 415–428], although the lagoon sediments contained four-fold higher THg concentrations. Conversely, the THg diffusive fluxes in the lagoon (up to 110 ng m−2 day−1) were one- to two-fold higher than those previously estimated for the Gulf of Trieste. The diurnal MeHg benthic fluxes were highest in summer at both sites (41,000 and 33,000 ng m−2 day−1 at the fishfarm and in the open lagoon, respectively), thus indicating the influence of temperature on microbial processes. The diurnal variations of dissolved THg and especially MeHg were positively correlated with O2 and inversely with DIC, suggesting an important influence of benthic photosynthetic activities on lagoon benthic Hg cycling, possibly through the production of organic matter promptly available for methylation. The results from the dark chamber incubated in the laboratory showed that the regeneration of dissolved THg was slightly affected by the oxic–anoxic transition. Conversely, the benthic flux of MeHg was up to 15-fold higher in sediments overlain by O2 depleted waters. In the anoxic phase, the MeHg fluxes proceeded in parallel with Fe fluxes and the methylated form reached approximately 100% of dissolved THg. The MeHg is mostly released into overlying water (mean recycling efficiency of 89%) until the occurrence of sulphide inhibition, due to scavenging of the available Hg substrate for methylation. The results suggest that sediments in the Grado Lagoon, especially during anoxic events, should be considered as a primary source of MeHg for the water column.  相似文献   

6.
To understand the geochemical cycle of Hg in hypereutrophic freshwater lake, two sampling campaigns were conducted in Lake Taihu in China during May and September of 2009. The concentrations of unfiltered total Hg (unfTHg) were in the range of 6.8–83 ng L−1 (28 ± 18 ng L−1) in the lake water and total Hg in the sediment was 12–470 ng g−1, both of which are higher than in other background lakes. The concentration of unfTHg in ∼11% of the lake water samples exceeded the second class of the Chinese environmental standards for surface water of 50 ng L−1 (GB 3838-2002), indicating that a high ecological risk is posed by the Hg in Lake Taihu. However, the concentrations of unfiltered total MeHg (unfMeHg) were relatively low in the lake water (0.14 ± 0.05 ng L−1, excluding two samples with 0.81 and 1.0 ng L−1). Lake sediment MeHg varied from 0.2–0.96 ng g−1, with generally low ratios of MeHg/THg of <1%. The low concentrations of TMeHg in the lake water may have resulted from a strong uptake by the high primary productivity and the demethylation of MeHg in oxic conditions. In addition, contrary to the results of previous research conducted in deep-water lakes and reservoirs, the low concentrations of MeHg and low ratio of MeHg/THg in the lake sediment indicates that the net methylation of Hg was not accelerated by the elevated organic matter load created by the eutrophication of Lake Taihu. The results also showed that sediments were a source of THg and MeHg in the water. Higher diffusion fluxes of THg and MeHg may be partly responsible for the higher concentrations of THg in the lake water in May, 2009.  相似文献   

7.
Concentrations of atmospheric Hg species, elemental Hg (Hg°), reactive gaseous Hg (RGM), and fine particulate Hg (Hg-PM2.5) were measured at a coastal site near Weeks Bay, Alabama from April to August, 2005 and January to May, 2006. Mean concentrations of the species were 1.6 ± 0.3 ng m−3, 4.0 ± 7.5 pg m−3 and 2.7 ± 3.4 pg m−3, respectively. A strong diel pattern was observed for RGM (midday maximum concentrations were up to 92.7 pg m−3), but not for Hg° or Hg-PM2.5. Elevated RGM concentrations (>25 pg m−3) in April and May of 2005 correlated with elevated average daytime O3 concentrations (>55 ppbv) and high light intensity (>500 W m−2). These conditions generally corresponded with mixed continental-Gulf and exclusively continental air mass trajectories. Generally lower, but still elevated, RGM peaks observed in August, 2005 and January–March, 2006 correlated significantly (p < 0.05) with peaks in SO2 concentration and corresponded to periods of high light intensity and lower average daytime O3 concentrations. During these times air masses were dominated by trajectories that originated over the continent. Elevated RGM concentrations likely resulted from photochemical oxidation of Hg° by atmospheric oxidants. This process may have been enhanced in and by the near-shore environment relative to inland sites. The marine boundary layer itself was not found to be a significant source of RGM.  相似文献   

8.
Mercury contained in buried landfill waste may be released via upward emission to the atmosphere or downward leaching to groundwater. Data from the US Geological Survey’s Amargosa Desert Research Site (ADRS) in arid southwestern Nevada reveal another potential pathway of Hg release: long-distance (102 m) lateral migration of elemental Hg (Hg0) through the unsaturated zone. Gas collected from multiple depths from two instrumented boreholes that sample the entire 110-m unsaturated zone thickness and are located 100 and 160 m away from the closest waste burial trench exhibit gaseous Hg concentrations of up to 33 and 11 ng m−3, respectively. The vertical distribution of gaseous Hg in the borehole closest to the disposal site shows distinct subsurface peaks in concentration at depths of 1.5 and 24 m that cannot be explained by radial diffusive transport through a heterogeneous layered unsaturated zone. The inability of current models to explain gaseous Hg distribution at the ADRS highlights the need to advance the understanding of gas-phase contaminant transport in unsaturated zones to attain a comprehensive model of landfill Hg release.  相似文献   

9.
The Xunyang Hg mine (XMM) situated in Shaanxi Province is an active Hg mine in China. Gaseous elemental Hg (GEM) concentrations in ambient air were determined to evaluate its distribution pattern as a consequence of the active mining and retorting in the region. Total Hg (HgT) and methylmercury (MeHg) concentrations in riparian soil, sediment and rice grain samples (polished) as well as Hg speciation in surface water samples were measured to show local dispersion of Hg contamination. As expected, elevated concentrations of GEM were found, ranging from 7.4 to 410 ng m−3. High concentrations of HgT and MeHg were also obtained in riparian soils, ranged from 5.4 to 120 mg kg−1 and 1.2 to 11 μg kg−1, respectively. Concentrations of HgT and MeHg in sediment samples varied widely from 0.048 to 1600 mg kg−1 and 1.0 to 39 μg kg−1, respectively. Surface water samples showed elevated HgT concentrations, ranging from 6.2 to 23,500 ng L−1, but low MeHg concentrations, ranging from 0.022 to 3.7 ng L−1. Rice samples exhibited high concentrations of 50–200 μg kg−1 in HgT and of 8.2–80 μg kg−1 in MeHg. The spatial distribution patterns of Hg speciation in the local environmental compartments suggest that the XMM is the source of Hg contaminations in the study area.  相似文献   

10.
Activity concentrations of the naturally occurring, short-lived and highly particle-reactive radionuclide tracer 234Th in the dissolved and particulate phase were determined at 7 shallow-water stations (maximum depths: 30 (S.1 and S.2), 65 (S.3), 97 (S.5), 105 (S.6) and 220 m (S.4 and S.7) in Saronikos Gulf and Elefsis Bay (central Aegean Sea, Greece) during 3 seasonal cruises (summer 2008, autumn 2008 and winter 2009) to assess the time scales of the dynamics and the depositional fate of particulate matter (POC, particulate 234Th). For that reason, in situ filtrating systems were deployed in several depths of the water column consisting of GF/A disc prefilters to scavenge particulate fraction of 234Th and organic carbon and impregnated cartridges to adsorb dissolved 234Th.The obtained data showed average particulate 234Th activity concentrations of 3.7 ± 0.4 Bq m−3 in summer, 2.1 ± 0.2 Bq m−3 in autumn and 2.4 ± 0.2 Bq m−3 in winter. The respective average dissolved 234Th activity concentrations were 30.1 ± 2.8 Bq m−3 in summer, 30.2 ± 2.9 Bq m−3 in autumn and 27.4 ± 3.0 Bq m−3 in winter. The activity ratios of total 234Th and its long-lived conservative parent 238U were below unity in most of the stations indicating radioactive disequilibrium throughout the water column, thus very dynamic trace-metal scavenging and particle export from the water column. These profiles (234Th and 238U) were used to estimate the export fluxes and scavenging rates of 234Th, as well as their residence times in the water column. The average cumulative export fluxes of particulate 234Th were estimated to be 33 ± 4 Bq m−2 d−1 in summer, 35 ± 5 Bq m−2 d−1 in autumn and 45 ± 6 Bq m−2 d−1 in winter, whereas the respective average cumulative scavenging rates of dissolved 234Th were 39 ± 5, 33 ± 5 and 50 ± 7 Bq m−2 d−1. Moreover, the cumulative average residence times of 234Th were 25 ± 4 d in summer, 45 ± 6 d in autumn and 64 ± 7 d in winter 2009 for the dissolved fraction and 4 ± 1, 3 ± 1 and 4 ± 1 d for the particulate one, respectively.POC/ ratio profiles decreased versus depth showing a variety of marine processes, such as loss of POC due to dissolution after biological activity, impact of minerals in particle sinking and microbial remineralization. Average cumulative export fluxes of POC were 162 ± 18 mmol m−2 d−1 in summer, 107 ± 19 mmol m−2 d−1 in autumn and 157 ± 25 mmol m−2 d−1 in winter 2009. The seasonal data of POC fluxes certified the existence of phytoplankton bloom in winter for Saronikos Gulf. In addition, after evaluating the maxima of POC fluxes in Elefsis Bay (a small embayment in northern Saronikos Gulf) during summer, potential bloom of phytoplankton also concluded; this approach is in agreement with previous data of the same area. Finally, the elevated POC concentrations and fluxes in the region certify that the Gulf is still one of the most organic polluted in the Mediterranean Sea.  相似文献   

11.
Monitoring of Hg in the atmosphere near volcanoes is limited with no previous data for Costa Rica. Seasonal and daily patterns of total gaseous mercury (TGM) were observed at the main sampling location at the Universidad Nacional, Heredia, Costa Rica. The area (lat. 10.000230 long. −84.109499) is located in the Central Valley of Costa Rica and is 27 km SE of the Poas volcano (lat. 10.199486 long. −84.231388). Measurements were made from May 2008 to May 2009 at this location with some additional values obtained at other sites near the Poas volcano including San Luis and Grecia as well as near, Turrialba and Irazu volcanoes. Total gaseous Hg was determined in samples collected at a height of 2 m using the Tekran 2537A (Tekran Inc.) gas-phase Hg vapor analyzer. Meteorological data (temperature, relative humidity, wind speed, wind direction, radiation and precipitation) were obtained from the airport weather station located at Alajuela. Monthly precipitation is typically 85 mm during the dry season (December to April) with winds from the west. The wet season begins in late April and continues to December with monthly rainfall of 328 mm and winds from the NE. The annual mean temperature is 20 °C. With the onset of the wet season TGM increased from typical values near 10 to 905 ng m−3. Measurements made within 5 km of the Poas volcano were higher than at Heredia at that time. Diel values measured at the university site increased until midday along with temperature and radiation. Relative humidity showed a reciprocal pattern. It was found that high values of TGM were not related to wind velocity or direction. The strong diel pattern increased with sunrise, peaked at midday and was lowest during the night time. It would seem that Hg0 from the volcano is oxidized and is deposited to the soils during the dry season when winds are blowing from the volcano. With the onset of heavy rains in April, Hg in the soil is reduced and re-volatilized resulting in the high levels in the atmosphere. Values at other volcano sites were provided. The role of atmospheric pollutants such as H2O2 and O3 should be included in future studies as they may result in oxidation of reduced Hg. The instability in the air masses may also be a factor and local pollution sources may result in high levels that is emitted from the volcanoes of Hg being circulated to ground level as radiation intensity increases.  相似文献   

12.
Mercury contamination of the environment is of worldwide concern because of its global presence and its potent neurotoxicity. Mining, smelting and the electronics industry are the main sources of Hg pollution. However, few studies have been performed to investigate systemic Hg contamination in metal mining regions. In this study, concentrations of Hg in air, farmland soil, and crops were measured in a Pb-Zn mining area in the karst region of Guangxi, China. Key factors that could affect Hg distribution, such as the fate of waste ore and waste residue, were analyzed. Geo-statistical methods were adopted to analyze the characteristics of spatial structure and distribution of Hg. The results show that Hg contamination in this region is serious. The total mercury (T-Hg) content is far higher than the Level II Limit Value of Chinese Soil Standards of 0.30 mg kg−1, showing obvious directional characteristics from WNW to ESE. Highest Hg concentrations were found in the WNW portion of the study area. The contamination of paddy soil is higher than that in dry farmland soil. The vertical distribution of T-Hg and its decrease with depth suggest that the important sources are waste water irrigation and the improper disposal of the waste ore and waste rock. The T-Hg concentrations in the agricultural products examined exceed the Chinese tolerance value (0.02 mg kg−1 for rice and 0.01 mg kg−1 for vegetables), indicating the seriousness of the problem. The ecological environment and the safety of food grown in this mining area are being affected, with the result that human health is possibly being affected.  相似文献   

13.
Few data are available on mercury (Hg) dynamics at high-elevation mountain sites. In this project, a whole-watershed approach was used to quantify major fluxes and pools of Hg in Sagehen basin, a closed basin in the Sierra Nevada mountains in California. Over a period spanning 9 months (January-September 2009), we estimated wet deposition inputs to the watershed at 3.8 μg m−2. Dry deposition added additional Hg in the range of 0.30-2.45 μg m−2 during this time period, and was the dominant deposition process during summer time. Seasonal snowpack accounted for only half of the Hg deposited by wet deposition. We suggest that photo-induced reduction of Hg(II) in snow and subsequent volatilization was responsible for this loss. Thus, snowpacks in the Sierra Nevada mountains likely reduce the effective atmospheric mercury flux via wet deposition due to significant emission fluxes prior to snowmelt. As such, wet Hg deposition could be of lesser importance as a Hg source in snow-dominated systems. Finally, stream runoff collected at the outlet of the watershed could account for only 4% of total Hg wet deposition suggesting that a large fraction of mercury deposition was sequestered in the ecosystem, specifically in the soils.  相似文献   

14.
The Wanshan Hg mining area in Guizhou, China, was one of the world’s largest Hg producing regions. Numerous mine-waste and calcines still remain, leaching Hg to local rivers and streams and potentially impacting the local population. Several studies have been published on local environmental impacts of these mining and retorting residues, but a comprehensive, regional survey on the distribution of Hg in the rivers in the region, as presented in this paper, has not previously been conducted. This study focuses on the regional distribution and temporal variation of aqueous Hg fractions in the five main watercourses draining the Wanshan Hg mining and retorting area, covering more than 700 km2. Three sampling campaigns were carried out in 2007 and 2008, covering high flow, normal flow and low flow periods. Total (THg), particulate (PHg), dissolved (DHg) and reactive (RHg) Hg fractions were determined. All rivers had the highest Hg concentrations at sample sites about 100–500 m downstream of the mine wastes. Total Hg concentrations ranged from extremely high (up to 12,000 ng L−1) at the sample site just 100 m below mine wastes, to quite low in tributary streams (1.9 ng L−1, about 14 km downstream of the mine wastes). Total Hg and PHg concentrations were usually highest during high flow periods in the Hg-contaminated areas (i.e. THg ? 50 ng L−1), while in the less-impacted downstream areas (with THg < 50 ng L−1) the Hg concentrations were usually lowest during high flow periods. Although highly elevated concentrations of Hg in water samples were found just downstream of the mine wastes, the concentrations decreased sharply to well below 50 ng L−1 (US EPA Hg concentration standard for protection of fresh water), within only 6–8 km downstream. Concentrations of THg were highly dominated by and correlated with PHg (R2 = 0.996–0.999, P < 0.001); PHg constituted more than 80% of THg in Hg-contaminated areas, and could account for 99.6% of the THg close to the mine wastes.  相似文献   

15.
Total particulate mercury (TPM) and reactive gaseous mercury (RGM) concentrations in ambient air on the eastern slope of the Mt. Gongga area, Sichuan Province, Southwestern China were monitored from 25 May, 2005 to 29 April, 2006. Simultaneously, Hg concentrations in rain samples were measured from January to December, 2006. The average TPM and RGM concentrations in the study site were 30.7 and 6.2 pg m−3, which are comparable to values observed in remote areas in Northern America and Europe, but much lower than those reported in some urban areas in China. The mean seasonal RGM concentration was slightly higher in spring (8.0 pg m−3) while the minimum mean concentration was observed in winter (4.0 pg m−3). TPM concentrations ranged across two orders of magnitude from 5.2 to 135.7 pg m−3 and had a clear seasonal variation: winter (74.1 pg m−3), autumn (22.5 pg m−3), spring (15.3 pg m−3) and summer (10.8 pg m−3), listed in decreasing order. The annual wet deposition was 9.1 μg m−2 and wet deposition in the rainy season (May–October) represented over 80% of the annual total. The temporal distribution of TPM and RGM suggested distinguishable dispersion characteristics of these Hg species on a regional scale. Elevated TPM concentration in winter was probably due to regional and local enhanced coal burning and low wet deposition velocity. The RGM distribution pattern is closely related to daily variation in UV radiation observed during the winter sampling period indicating that photo-oxidation processes and diurnal changes in meteorology play an important role in RGM generation.  相似文献   

16.
Methane and CO2 emissions from the two most active mud volcanoes in central Japan, Murono and Kamou (Tokamachi City, Niigata Basin), were measured in from both craters or vents (macro-seepage) and invisible exhalation from the soil (mini- and microseepage). Molecular and isotopic compositions of the released gases were also determined. Gas is thermogenic (δ13CCH4 from −32.9‰ to −36.2‰), likely associated with oil, and enrichments of 13C in CO2 (δ13CCO2 up to +28.3‰) and propane (δ13CC3H8 up to −8.6‰) suggest subsurface petroleum biodegradation. Gas source and post-genetic alteration processes did not change from 2004 to 2010. Methane flux ranged within the orders of magnitude of 101-104 g m−2 d−1 in macro-seeps, and up to 446 g m−2 d−1 from diffuse seepage. Positive CH4 fluxes from dry soil were widespread throughout the investigated areas. Total CH4 emission from Murono and Kamou were estimated to be at least 20 and 3.7 ton a−1, respectively, of which more than half was from invisible seepage surrounding the mud volcano vents. At the macro-seeps, CO2 fluxes were directly proportional to CH4 fluxes, and the volumetric ratios between CH4 flux and CO2 flux were similar to the compositional CH4/CO2 volume ratio. Macro-seep flux data, in addition to those of other 13 mud volcanoes, supported the hypothesis that molecular fractionation (increase of the “Bernard ratio” C1/(C2 + C3)) is inversely proportional to gas migration fluxes. The CH4 “emission factor” (total measured output divided by investigated seepage area) was similar to that derived in other mud volcanoes of the same size and activity. The updated global “emission-factor” data-set, now including 27 mud volcanoes from different countries, suggests that previous estimates of global CH4 emission from mud volcanoes may be significantly underestimated.  相似文献   

17.
Recent Lake Tanganyika Hg deposition records were derived using 14C and excess 210Pb geochronometers in sediment cores collected from two contrasting depositional environments: the Kalya Platform, located mid-lake and more removed from watershed impacts, and the Nyasanga/Kahama River delta region, located close to the lake’s shoreline north of Kigoma. At the Kalya Platform area, pre-industrial Hg concentrations are 23 ± 0.2 ng/g, increasing to 74 ng/g in modern surface sediment, and the Hg accumulation rate has increased from 1.0 to 7.2 μg/m2/a from pre-industrial to present, which overall represents a 6-fold increase in Hg concentration and accumulation. At the Nyasanga/Kahama delta region, pre-industrial Hg concentrations are 20 ± 3 ng/g, increasing to 46 ng/g in surface sediment. Mercury accumulation rate has increased from 30 to 70 μg/m2/a at this site, representing a 2–3-fold increase in Hg concentration and accumulation. There is a lack of correlation between charcoal abundance and Hg accumulation rate in the sediment cores, demonstrating that local biomass burning has little relationship with the observed Hg concentration or Hg accumulation rates. Examined using a sediment focusing-corrected mass accumulation rate approach, the cores have similar anthropogenic atmospheric Hg deposition profiles, suggesting that after accounting for background sediment concentrations the source of accumulating Hg is predominantly atmospheric in origin. In summary, the data document an increase of Hg flux to the Lake Tanganyika ecosystem that is consistent with increasing watershed sediment delivery with background-level Hg contamination, and regional as well as global increases in atmospheric Hg deposition.  相似文献   

18.
We report the application of an in situ method to obtain field dissolution rates of fine mineral particles in soils. Samples with different metal-containing mineral and slag particles (lead oxide, copper concentrate and copper slag) from the mining and smelting industry were buried in the topsoil of an acidic forest soil for up to 18 months. In addition we studied the dissolution of these particles in samples of the same soil, in a sand matrix and in acid solution under constant temperature and moisture conditions in the laboratory. Under field conditions the PbO particles dissolved quite rapidly (2.4 ± 0.7 × 10−10 mol Pb m−2 s−1), whereas the copper concentrate (<1 × 10−11 mol Cu m−2 s−1) and the copper slag particles (4.3 ± 0.8 × 10−11 mol Cu m−2 s−1) proved to be more resistant to weathering. In addition to qualitative information on dissolution features (SEM), the method yielded quantitative data on in situ dissolution rates. The dissolution rates followed the order: sand with acid percolation (pH 3.5; lab) < soil (lab) < soil (field) < acid solution (pH 3.5; lab). Dissolution rates in soil were found to be lower under laboratory than under field conditions. The faster field rates may in part be attributed to the higher biological activity in the field soil compared to the same soil in the laboratory.  相似文献   

19.
The continental shelf benthic iron flux and its isotope composition   总被引:1,自引:0,他引:1  
Benthic iron fluxes from sites along the Oregon-California continental shelf determined using in situ benthic chambers, range from less than 10 μmol m−2 d−1 to values in excess of ∼300 μmol m−2 d−1. These fluxes are generally greater than previously published iron fluxes for continental shelves contiguous with the open ocean (as opposed to marginal seas, bays, or estuaries) with the highest fluxes measured in the regions around the high-sediment discharge Eel River and the Umpqua River. These benthic iron fluxes do not covary with organic carbon oxidation rates in any systematic fashion, but rather seem to respond to variations in bottom water oxygen and benthic oxygen demand. We hypothesize that the highest rates of benthic iron efflux are driven, in part, by the greater availability of reactive iron deposited along these river systems as compared to other more typical continental margin settings. Bioirrigation likely plays an important role in the benthic Fe flux in these systems as well. However, the influence of bottom water oxygen concentrations on the iron flux is significant, and there appears to be a threshold in dissolved oxygen (∼60-80 μM), below which sediment-ocean iron exchange is enhanced. The isotope composition of this shelf-derived benthic iron is enriched in the lighter isotopes, and appears to change by ∼3‰ (δ56Fe) during the course of a benthic chamber experiment with a mean isotope composition of −2.7 ± 1.1‰ (2 SD, n = 9) by the end of the experiment. This average value is slightly heavier than those from two high benthic Fe flux restricted basins from the California Borderland region where δ56Fe is −3.4 ± 0.4‰ (2 SD, n = 3). These light iron isotope compositions support previous ideas, based on sediment porewater analyses, suggesting that sedimentary iron reduction fractionates iron isotopes and produces an isotopically light iron pool that is transferred to the ocean water column. In sum, our data suggest that continental shelves may export a higher efflux of iron than previously hypothesized, with the likelihood that along river-dominated margins, the benthic iron flux could well be orders of magnitude larger than non-river dominated shelves. The close proximity of the continental shelf benthos to the productive surface ocean means that this flux is likely to be essential for maintaining ecosystem micronutrient supply.  相似文献   

20.
Aqueous production and water-air exchange of elemental mercury (Hg0) are important features of the environmental cycling of Hg. We investigated Hg0 cycling in ten Arctic Alaskan lakes that spanned a wide range in physicochemical characteristics. Dissolved gaseous Hg (DGM, dominated by Hg0) varied from 40 to 430 fM and averaged 200 fM. All surface waters were supersaturated relative to the atmosphere. DGM averaged 3 ± 2% of dissolved (i.e., filter passing) dissolved total mercury (DTM) and 15 ± 6% of dissolved labile Hg (DLM). In-lake DGM profiles generally followed the vertical distribution of light, indicating photoreduction of Hg(II) complexes as a source of Hg0. Additionally, DGM correlated linearly with DLM (r2 = 0.82, p < 0.0001) in the lake surface, signifying that Hg complexes (mostly organic Hg associations) in dissolved phase are photoreducible and contribute to production of DGM. Further, a positive relation between DGM/DTM and both Ka (light attenuation coefficient; r2 = 0.73, p < 0.02) and DOC (r2 = 0.60, p = 0.02) suggests that solar radiation and dissolved organic matter control DGM production and its cycling. An average rate of DGM formation (0.6 ± 0.2% of DTM d−1; range, 0.20.8) was estimated by assuming steady state with the evasional rate. In-lake DGM formation occurs at lower rates in waters with greater suspended particulate matter and dissolved organic carbon (DOC), pointing to the significant role of organic matter plays in controlling DGM formation in these aquatic systems. Estimated evasional fluxes of Hg0 (average, 140 ± 50 pmol m−2 d−1; range, 60-200) were comparable to those of temperate lakes (e.g., Wisconsin, Michigan). In arctic lakes, the rate of evasion during ice-free periods (7 ± 3 nmol m−2 yr−1) is similar to the atmospheric input of Hg (wet + dry) to the lakes based on levels in summertime precipitation but not including additional sources, e.g., springtime depletion.  相似文献   

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