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1.
Jiang S  Liu X  Chen Q 《Chemosphere》2011,83(8):1108-1116
The toxicities and bioavailabilities of total mercury (THg) and methylmercury (MeHg) in aquatic systems have made them the subjects of recent research. In this study, we collected a lake sediment core from Ny-Ålesund in Svalbard and analyzed the distributions of THg and MeHg in the sediments. The increased trend of THg was caused by anthropogenic contamination since the 14th century through long-range transportation, especially after the industrial era. However, the peak values of Hg in surface sediment samples could be explained by the increased algal scavenging process in recent decades. All the biogeochemical proxies (e.g., pigments and diatom biomass) revealed recent sharp increases in aquatic primary production due to the current climate warming. Rock-Eval analyses indicated that algal-derived organic matter took up a large portion, and quantitative calculation showed that 89.6-95.8% of the Hg in post-1950 could be explained by scavenging. The distribution of MeHg has a close relationship with total Hg and organic matter. The oxidation-reduction condition is one of the possible factors affecting the methylation rates in H2 lake sediments. Higher algal productivity and organic matter actually led to the increased trend of methylation in the uppermost sediment. This study supports some new key hypotheses on climate-driven factors affecting Hg and MeHg cycling in High Arctic lake sediments.  相似文献   

2.
Six groups participated in an international study of springtime atmospheric mercury depletion events (AMDEs) at Ny-Ålesund in the Norwegian Arctic during April and May 2003 with the aim to compare analytical methods for measurements of atmospheric mercury species and study the physical and chemical processes leading to AMDEs. Five groups participated in the method comparison that was conducted at three different locations within Ny-Ålesund. Various automated and manual instrumentation were used to sample, measure and compare gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and mercury associated with particles (Hg-P). The concentration of GEM was reproducible during background conditions. For the first time using ambient air, the statistics associated with round robin test procedures were applied. This was found to be an appropriate tool to investigate the reproducibility of GEM measurements in ambient air. The precision for each group measuring GEM concentrations was found to be consistently good (within 5%). Five AMDEs were recorded during the study. Using four different methods, including single and replicate samples, all groups recorded higher values of RGM and Hg-P during AMDEs. The results show that measuring comparable atmospheric mercury species at both the same and different locations (within the Ny-Ålesund area) is difficult. Not only do site location and site characteristics create challenges when trying to intercompare results but there are difficulties, as well, in obtaining comparable results with similar sampling and analysis methods. Nevertheless, with our current procedures for atmospheric mercury identification we can differentiate with certainty between “high” and “low” concentration values of RGM and Hg-P.  相似文献   

3.
PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) samples (n = 58) collected every sixth day in Xi’an, China, from 5 July 2008 to 27 June 2009 are analyzed for levoglucosan (1,6-anhydro-β-d-glucopyranose) to evaluate the impacts of biomass combustion on ambient concentrations. Twenty-four-hour levoglucosan concentrations displayed clear summer minima and winter maxima that ranged from 46 to 1889 ng m?3, with an average of 428 ± 399 ng m?3. Besides agricultural burning, biomass/biofuel combustion for household heating with straws and branches appears to be of regional importance during the heating season in northwestern China. Good correlations (0.70 < R < 0.91) were found between levoglucosan relative to water-soluble K+, Cl?, organic carbon (OC), elemental carbon (EC), and glyoxal. The highest levoglucosan/OC ratio of 2.3% was found in winter, followed by autumn (1.5%). Biomass burning contributed to 5.1–43.8% of OC (with an average of 17.6 ± 8.4%).

Implications:?PM2.5 levoglucosan concentrations and the correlation between levoglucosan relative to other compounds during four seasons in Xi’an showed that the influence of biomass burning is maximum during the residential heating season (winter), although some important influences may be detected in spring (field preparation burnings) and autumn (corn stalks and wheat straw burning, fallen dead leaves burning) at Xi’an and surrounding areas. Household heating with biomass during winter was quite widespread in Guanzhong Plain. Therefore, the control of biomass/biofuel combustion could be an effective method to reduce pollutant emission on a regional scale.  相似文献   

4.
Distribution of mercury in the aquatic environment at Almadén,Spain   总被引:1,自引:0,他引:1  
The world's largest mercury mine is placed at Almadén, Spain. However, there is a lack of information about the environmental impact of these mining activities in the ecosystem that surrounds this area. The aim of this article is to document the concentration of mercury in waters, sediments and bivalves of the aquatic system impacted by historic mine wastes. Simultaneously, a comprehensive study has been undertaken to characterise this hydrosystem and to determine the influence of some major physico-chemical parameters on the fate of mercury. Samplings were carried out for the last few years. Concentration of mercury in waters ranged from not detectable to 20 microg/l. For the sediments study, samples have been taken both from contaminated and non-contaminated sites within the basin. The regional background mercury concentration is higher than values typically cited for natural backgrounds. At exposed sites the mercury concentrations between 5 and 1000 microg/g were measured. These values are one to four order of magnitude greater than regional background levels. In the comparison between the results obtained at the present moment and those available for the 1974-1977 period, a general diminution of mercury levels is observed. Mercury concentrations in fresh water bivalves ranged between 1 and 4 microg/g (d.w.), with around 30% as monomethylmercury. In the discussion of the implications for risk assessment data available for other areas affected both for mine activities and mercuriferous belt are included.  相似文献   

5.
We use GEOS-Chem chemical transport model simulations of sulfate–ammonium aerosol data from the NASA ARCTAS and NOAA ARCPAC aircraft campaigns in the North American Arctic in April 2008, together with longer-term data from surface sites, to better understand aerosol sources in the Arctic in winter–spring and the implications for aerosol acidity. Arctic pollution is dominated by transport from mid-latitudes, and we test the relevant ammonia and sulfur dioxide emission inventories in the model by comparison with wet deposition flux data over the source continents. We find that a complicated mix of natural and anthropogenic sources with different vertical signatures is responsible for sulfate concentrations in the Arctic. East Asian pollution influence is weak in winter but becomes important in spring through transport in the free troposphere. European influence is important at all altitudes but never dominant. West Asia (non-Arctic Russia and Kazakhstan) is the largest contributor to Arctic sulfate in surface air in winter, reflecting a southward extension of the Arctic front over that region. Ammonium in Arctic spring mostly originates from anthropogenic sources in East Asia and Europe, with added contribution from boreal fires, resulting in a more neutralized aerosol in the free troposphere than at the surface. The ARCTAS and ARCPAC data indicate a median aerosol neutralization fraction [NH4+]/(2[SO42?] + [NO3?]) of 0.5 mol mol?1 below 2 km and 0.7 mol mol?1 above. We find that East Asian and European aerosol transported to the Arctic is mostly neutralized, whereas West Asian and North American aerosol is highly acidic. Growth of sulfur emissions in West Asia may be responsible for the observed increase in aerosol acidity at Barrow over the past decade. As global sulfur emissions decline over the next decades, increasing aerosol neutralization in the Arctic is expected, potentially accelerating Arctic warming through indirect radiative forcing and feedbacks.  相似文献   

6.
In order to assess the temporal variabilities of atmospheric mercury (Hg) from an area moderately impacted by man-made source processes, the concentrations of total gaseous mercury were measured routinely from an urban monitoring station during January 1999–August 2000. The mean hourly concentration of Hg from overall measurements was computed to be 5.26±3.27 ng m−3 (N=11, 572). Using these measurement data, we inspected various aspects on the temporal distribution of Hg. When analyzed over 24 h scale, the pattern was characterized by high concentration during nighttime relative to daytime (e.g., values approaching 9 ng m−3). This pattern was prominent during winter and seen persistently across fall, spring, and summer. When divided seasonally, the highest mean of 6.01 ng m−3 was observed during winter. It appears that such wintertime dominance is most likely to come from the anthropogenic sources such as household heating systems from late fall to early spring. A close inspection of the Hg data however indicated that the seasonal variation proceeded quite dynamically. Inspection of seasonally divided data groups generally showed substantial variabilities among different months. In order to analyze the factors affecting Hg distributions over different time scale, we conducted the correlation analysis. Whereas Hg generally exhibited strong correlations with such parameters as PM, SO2, and NO2, its relationship varied diurnally and seasonally. The overall results of the present study suggest that changes in its source signatures can vary over varying time scale under the influence of strong man-made source processes.  相似文献   

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One of the most critical measurements needed to understand the biogeochemical cycle of mercury, and to verify atmospheric models, is the rate of mercury wet-deposition. The Mercury Deposition Network (MDN) operates sites across North America to monitor total mercury in wet-deposition. MDN's primary goal is to provide both spatial and temporal continental-scale observations of mercury wet-deposition fluxes to support researchers, modelers, policy-makers and the public interest. MDN represents the only continental-scale mercury deposition database with a >10-year record of continuous values. This study provides analysis and interpretation of MDN observations at 10 years (1996–2005) with an emphasis on investigating whether rigorous, statistically-significant temporal trends and spatial patterns were present and where they occurred. Wet deposition of mercury ranges from more than 25 μg m?2 yr in south Florida to less than 3 μg m?2 yr in northern California. Volume-weighted total mercury concentrations are statistically different between defined regions overall (Southeast ≈ Midwest > Ohio River > Northeast), with the highest in Florida, Minnesota, and several Southwest locations (10–16 ng L?1). Total mercury wet-deposition is significantly different between defined regions (Southeast > Ohio River > Midwest > Northeast). Mercury deposition is strongly seasonal in eastern North America. The average mercury concentration is about two times higher in summer than in winter, and the average deposition is approximately more than three times greater in summer than in winter. Forty-eight sites with validated datasets of five years or more were tested for trends using the non-parametric seasonal Kendall trend test. Significant decreasing mercury wet-deposition concentration trends were found at about half of the sites, particularly across Pennsylvania and extending up through the Northeast.  相似文献   

9.
Sediments from the Castilseras reservoir, located downstream on the Valdeazogues River in the Almadén mercury district, were collected to assess the potential contamination status related to metals(oids) associated with river sediment inputs from several decommissioned mines. Metals(oids) concentrations in the reservoir sediments were investigated using different physical and chemical techniques. The results were analyzed by principal component analysis (PCA) to explain the correlations between the sets of variables. The degree of contamination was evaluated using the enrichment factor (EF) and the geoaccumulation index (Igeo). PCA revealed that the silty fraction is the main metals(oids) carrier in the sediments. Among the potentially harmful elements, there is a group (Al, Cr, Cu, Fe, Mn, Ni, and Zn) that cannot be strictly correlated to the mining activity since their concentrations depend on the lithological and edaphological characteristics of the materials. In contrast, As, Co, Hg, Pb, and S showed significant enrichment and contamination, thus suggesting relevant contributions from the decommissioned mines through fluvial sediment inputs. As far as Hg and S are concerned, the high enrichment levels pose a question concerning the potential environmental risk of transfer of the organic forms of Hg (mainly methylmercury) from the bottom sediments to the aquatic food chain.  相似文献   

10.
In the shallow environment, the nutrient and carbon exchanges at the sediment–water interface contribute significantly to determine the trophic status of the whole water column. The intensity of the allochthonous input in a coastal environment subjected to strong anthropogenic pressures determines an increase in the benthic oxygen demand leading to depressed oxygen levels in the bottom waters. Anoxic conditions resulting from organic enrichment can enhance the exchange of nutrients between sediments and the overlying water. In the present study, carbon and nutrient fluxes at the sediment–water interface were measured at two experimental sites, one highly and one moderately contaminated, as reference point. In situ benthic flux measurements of dissolved species (O2, DIC, DOC, N-NO3 ?, N-NO2 ?, N-NH4 +, P-PO4 3?, Si-Si(OH)4, H2S) were conducted using benthic chambers. Furthermore, undisturbed sediment cores were collected for analyses of total and organic C, total N, and biopolymeric carbon (carbohydrates, proteins, and lipids) as well as of dissolved species in porewaters and supernatant in order to calculate the diffusive fluxes. The sediments were characterized by suboxic to anoxic conditions with redox values more negative in the highly contaminated site, which was also characterized by higher biopolymeric carbon content (most of all lipids), lower C/N ratios and generally higher diffusive fluxes, which could result in a higher release of contaminants. A great difference was observed between diffusive and in situ benthic fluxes suggesting the enhancing of fluxes by bioturbation and the occurrence of biogeochemically important processes at the sediment–water interface. The multi-contamination of both inorganic and organic pollutants, in the sediments of the Mar Piccolo of Taranto (declared SIN in 1998), potentially transferable to the water column and to the aquatic trophic chain, is of serious concern for its ecological relevance, also considering the widespread fishing and mussel farming activities in the area.  相似文献   

11.
The study aimed to assess morphological, structural and compositional alterations in Scrobicularia plana nacre environmentally exposed to mercury in order to seek out the possibility of the assessed alterations as a monitoring tool to handle complexity and interactions of metals in the environment involving a non-invasive methodology. Bivalves were collected from a mercury contaminated site (Laranjo basin – Ria de Aveiro, Portugal) and a reference site in the same aquatic system. The combination of scanning electron microscopy (SEM) with energy-dispersive X-ray spectroscopy (EDS) technique depicted a sheet like morphology of bivalve nacre collected from the reference site. Moreover, EDS plot exhibited the presence of potassium, oxygen, calcium, and carbon elements. Shells collected from the contaminated area depicted lamellar patches like structures with particle like morphology composition. SEM images corresponding to the elemental analysis by EDS plot clearly denoted the presence of mercury. SEM images from the other locations of the contaminated shells depicted large surface area, a broken or ruptured symmetry of organic matrix as well as crack-like gaps. The influence of environmental mercury affecting the surface morphology of S. plana nacre showed dimple like morphology (as proved by transmission electron microscopy, TEM). The possible explanation may be the replacement of calcium elements with other elements or alloys from the nacre composite collected from contaminated region. Therefore, the nacre fingerprint may be useful as innovative knowledge and applicable tool aiming at risk reduction from noxious mercury present in the environment. Overall results suggested the use of shell as an indelible fingerprint of metal exposure.  相似文献   

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A large copper–nickel smelter complex is located at the Kole Penninsula, Russia, close to the Norwegian border. Trace-element concentrations in surface sediments (0–0.5 cm) and pre-industrial sediments from 45 lakes in the region were used to uncover spatial deposition patterns and contamination factor of sediments. Elevated concentrations were found, especially for Ni and Cu, but also for Pb, Co, Hg, As, and Cd. Highest concentrations were found up to 20 km from the smelter, but the concentrations decreased exponentially with distance from the smelter. Increasing Ni, Cu, As, and Hg concentrations from sub-surface to surface sediments were found for lakes at intermediate distances (20–60 km). This may reflect recent changes in atmospheric depositions, as shown in nearby Norwegian areas. However, we cannot rule out that this also may have been caused by diagenetic processes, especially for the most redox-sensitive elements such as As.  相似文献   

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Environmental Science and Pollution Research - Diet is an important exposure pathway of phthalate esters (PAEs) for humans. A total of 174 food samples covering 11 food groups were collected from...  相似文献   

15.

An appraisal of seawater intrusion into the coastal aquifers is one of the major issues for groundwater resource management. The GALDIT model applies to the analysis of multiple parameters using systematic GIS techniques for mapping and assessment of seawater intrusion vulnerability. It demarcates the mapping of potential vulnerability that shows a higher vulnerability to seawater intrusion in various parts of the coast and the estimated vulnerability index value of 7.50 and 9.64. An area of 33.0 km2 spread in the low-lying coastal area comprising estuaries, salt marshes, and saltpans shows the high vulnerability condition with an estimated vulnerability value of 6.42–7.50. An area of 73.20 km2 spread over coastal and alluvial plains experiences moderate vulnerability (temporal salinity in the groundwater sources) with an estimated vulnerability index value of 5.46–6.42. Aquifers underlying coastal uplands (hard rock formations) and some parts of accretionary beaches (2.05 km2) are relatively protected fresh groundwater sources, wherein the estimated vulnerability index is 4.55–5.46. The vulnerability mapping of the GALDIT model using hydrochemical analysis of primary groundwater parameters such as TDS, Cl?, HCO3, and Cl?/HCO3 ratio is validated. Higher concentration of TDS (2637–4162 mg/l) and Cl? (1268–2347 mg/l) is taken for the areas falling under higher vulnerability to seawater intrusion, especially in the placer mining sites and coastal areas facing erosion. Similarly, the groundwater sources of the low-lying areas including estuaries, salt marshes, saltpans, and backwater were noted to have higher values of Cl?/HCO3 with a rationality of 9.87–12.18. Hydrological facies shows the highest concentration of NaCl in the groundwater sources within the proximity of eroded beaches, saltwater bodies, and sand mining areas. A hydrochemical facies evolution (HFE) diagram represents the hydrochemical facies of groundwater elements that shows an intrusion of seawater into the coastal aquifers underlying the very high vulnerable zones. Higher bicarbonate concentration (233–318 mg/l) is noticed in the upland areas and some parts of dunes and accreted beaches, sandy coasts, and uplands. Vulnerability analysis reveals that those areas near saltwater bodies and eroding coasts are prone to lateral and vertical diffusion of saltwater. The geodatabase developed through such modeling studies can help in planning and developing activities for sustainable groundwater resource management in coastal areas.

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16.
This study characterizes over 5 years of high time resolution (5 min), airborne black carbon (BC) concentrations (July 2003 to December 2008) measured over Ahmedabad, an urban region in western India. The data were used to obtain different time averages of BC concentrations, and these averages were then used to assess the diurnal, seasonal, and annual variability of BC over the study region. Assessment of diurnal variations revealed a strong association between BC concentrations and vehicular traffic. Peaks in BC concentration were co-incident with the morning (0730 to 0830, LST) and late evening (1930 to 2030, LST) rush hour traffic. Additionally, diurnal variability in BC concentrations during major festivals (Diwali and Dushera during the months of October/November) revealed an increase in BC concentrations due to fireworks displays. Maximum half hourly BC concentrations during the festival days were as high as 79.8 μg m?3. However, the high concentrations rapidly decayed suggesting that local meteorology during the festive season was favorable for aerosol dispersion. A multiple linear regression (MLR) model with BC as the dependent variable and meteorological parameters as independent variables was fitted. The variability in temperature, humidity, wind speed, and wind direction accounted for about 49% of the variability in measured BC concentrations. Conditional probability function (CPF) analysis was used to identify the geographical location of local source regions contributing to the effective BC measured (at 880 nm) at the receptor site. The east north-east (ENE) direction to the receptor was identified as a major source region. National highway (NH8) and two coal-fired thermal power stations (at Gandhinagar and Sabarmati) were located in the identified direction, suggesting that local traffic and power plant emissions were likely contributors to the measured BC.  相似文献   

17.
The performance of various algal indices to document improvements in water quality across a low nutrient concentration gradient was assessed during 2 years in the St Lawrence River (Quebec, Canada). Water-quality variables and periphyton samples were collected on navigational buoys near Montreal during the spring, summer and fall of 1994 and 1995. Exposure to urban wastewater varied widely within the sector surrounding the island of Montreal, with some areas upstream receiving no direct effluents and areas further downstream receiving treated and untreated wastewater. Faecal coliform concentrations provided a good tracer of effluents and were significantly correlated to nutrient concentrations (r = 0.33-0.72, p < 0.001) and water transparency (r = 0.70, p < 0.001). Despite a strong gradient in faecal coliform concentration (< 2 to > 20 000 UFC/100 ml), algal biomass and diversity did not reflect differences between sites with varying levels of urban wastewater. Taxonomic composition of periphyton communities, particularly the presence of the cyanophyte Plectonema notatum Schmidle, was related (r = 0.48, p = 0.004) to exposure to urban effluents. Variables describing seasonal changes (temperature, Julian day, river discharge, conductivity, NO2-NO3) explained a large fraction of total variance (38-52% of total variance) and thus exerted the predominant influence on algal biomass and species composition in the St Lawrence River. Variables describing the presence of effluents explained 1-22% of the variance in compositional data. Subtle changes in periphyton species composition were the only response to different levels of exposure to urban wastewater in the Montreal area, which represented relatively small differences in comparison to natural seasonal variability.  相似文献   

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