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1.
Atmospheric elemental, reactive and particulate mercury (Hg) concentrations were measured north of downtown Reno, Nevada, USA from November 2004 to November 2007. Three-year mean and median concentrations for gaseous elemental Hg (Hg0) were 1.6 and 1.5 ng m−3 (respectively), similar to global mean Hg0 concentrations. The three-year mean reactive gaseous Hg (RGM) concentration (26 pg m−3) was higher than values reported for rural sites across the western United States. Well defined seasonal and daily patterns in Hg0 and RGM concentrations were observed, with the highest Hg0 concentrations measured in winter and early morning, and RGM concentrations being greatest in the summer and mid-afternoon. Elevated Hg0 concentrations in winter were associated with periods of cold, stagnant air; while a regularly observed early morning increase in concentration was due to local source and surface emissions. The observed afternoon increase and high summer values of RGM can be explained by in situ oxidation of gaseous Hg0 or mixing of RGM derived from the free troposphere to the surface. Because both of these processes are correlated with the same environmental conditions it is difficult to assess their overall contribution to the observed trends.  相似文献   

2.
In China, total Hg (HgT) and methylmercury (MeHg) were quantified in rice grain grown in three sites using water-saving rice cultivation methods, and in one Hg-contaminated site, where rice was grown under flooded conditions. Polished white rice concentrations of HgT (water-saving: 3.3 ± 1.6 ng/g; flooded: 110 ± 9.2 ng/g) and MeHg (water-saving 1.3 ± 0.56 ng/g; flooded: 12 ± 2.4 ng/g) were positively correlated with root-soil HgT and MeHg contents (HgT: r2 = 0.97, MeHg: r2 = 0.87, p < 0.05 for both), which suggested a portion of Hg species in rice grain was derived from the soil, and translocation of Hg species from soil to rice grain was independent of irrigation practices and Hg levels, although other factors may be important. Concentrations of HgT and other trace elements were significantly higher in unmilled brown rice (p < 0.05), while MeHg content was similar (p > 0.20), indicating MeHg infiltrated the endosperm (i.e., white rice) more efficiently than inorganic Hg(II).  相似文献   

3.
We evaluated the Danish AirGIS air quality and exposure model system using air quality measurement data from New York City in the Multi-Ethnic Study of Atherosclerosis and Air Pollution (MESA Air). Measurements were used from three US EPA Air Quality System (AQS) monitoring stations and a comprehensive MESA Air measurement campaign including about 150 different locations and about 650 samples of about 2 week measurements of NOx, NO2 and PM2.5. AirGIS is a deterministic exposure model system based on the dispersion models Operational Street Pollution Model (OSPM) and the Urban Background Model (UBM). The UBM model reproduced the annual levels within 1–26% depending on station and pollutant at the three urban background EPA monitor stations, and generally reproduced well the seasonal and diurnal variation. The full model with OSPM and UBM reproduced the MESA Air measurements with a correlation coefficient of r2 = 0.51 for NOx, r2 = 0.28 for NO2 and r2 = 0.73 for PM2.5.  相似文献   

4.
Chlordecone is a toxic organochlorine insecticide that was used in banana plantations until 1993 in the French West Indies. This study aimed at assessing the potential of near infrared reflectance spectroscopy (NIRS) for determining chlordecone content in Andosols, Nitisols and Ferralsols from Martinique. Using partial least square regression, chlordecone content conventionally determined through gas chromatography–mass spectrometry could be correctly predicted by NIRS (Q2 = 0.75, R2 = 0.82 for the total set), especially for samples with chlordecone content <12 mg kg−1 or when the sample set was rather homogeneous (Q2 = 0.91, R2 = 0.82 for the Andosols). Conventional measures and NIRS predictions were poorly correlated for chlordecone content >12 mg kg−1, nevertheless ca. 80% samples were correctly predicted when the set was divided into three or four classes of chlordecone content. Thus NIRS could be considered a time- and cost-effective method for characterising soil contamination by chlordecone.  相似文献   

5.
Hg species (total mercury, methylmercury, reactive mercury) in precipitation were investigated in the vicinity of the Lehigh Hanson Permanente Cement Plant in the San Francisco Bay Area, CA., USA. Precipitation was collected weekly between November 29, 2007 and March 20, 2008, which included the period in February and March 2008 when cement production was minimized during annual plant maintenance. When the cement plant was operational, the volume weighted mean (VWM) and wet depositional flux for total Hg (HgT) were 6.7 and 5.8 times higher, respectively, compared to a control site located 3.5 km east of the cement plant. In February and March, when cement plant operations were minimized, levels were approximately equal at both sites (the ratio for both parameters was 1.1). Due to the close proximity between the two sites, meteorological conditions (e.g., precipitation levels, wind direction) were similar, and therefore higher VWM HgT levels and HgT deposition likely reflected increased Hg emissions from the cement plant. Methylmercury (MeHg) and reactive Hg (Hg(II)) were also measured; compared to the control site, the VWM for MeHg was lower at the cement plant (the ratio = 0.75) and the VWM for Hg(II) was slightly higher (ratio = 1.2), which indicated the cement plant was not likely a significant source of these Hg species to the watershed.  相似文献   

6.
Concentrations of 55 volatile organic compounds (VOCs) (C2–C12) are reported near a highway in Raleigh, NC. Thirty-minute samples were collected at eight locations, ranging from approximately 10–100 m perpendicular from the roadway. The highest concentrations of VOCs were generally measured closest to the roadway, and concentrations decreased exponentially with increasing distance from the roadway. The highest mean concentration for individual VOCs were for ethylene (3.10 ppbv) (mean concentration at x = 13 m), propane (2.27 ppbv), ethane (1.91 ppbv), isopentane (1.54 ppbv), toluene (0.95 ppbv), and n-butane (0.89 ppbv). Concentrations at the nearest roadway location (x = 13 m) were generally between 2.0 and 1.5 times those from the farthest roadway location (x = 92 m). The data were apportioned into four source categories using the EPA Chemical Mass Balance Model (CMB8.2): motor vehicle exhaust, compressed natural gas, propane gas, and evaporative gasoline. The majority of the VOCs resulted from motor vehicle exhaust (67 ± 12%) (% of total VOC at x = 13 m ± S.D.). Compressed natural gas, propane gas, and evaporative gasoline accounted for approximately 15%, 7% and 1% of the total VOC emissions, respectively, at x = 13 m.  相似文献   

7.
The status of the current knowledge concerning the dry deposition of atmospheric mercury, including elemental gaseous mercury (Hg0), reactive gaseous mercury (RGM), and particulate mercury (Hgp), is reviewed. The air–surface exchange of Hg0 is commonly bi-directional, with daytime emission and nighttime deposition over non-vegetated surfaces and vegetated surfaces with small leaf area indices under low ambient Hg0 conditions. However, daytime deposition has also been observed, especially when the ambient Hg0 is high. Typical dry deposition velocities (Vd) for Hg0 are in the range of 0.1–0.4 cm s?1 over vegetated surfaces and wetlands, but substantially smaller over non-vegetated surfaces and soils below canopies. Meteorological, biological, and soil conditions, as well as the ambient Hg0 concentrations all play important roles in the diurnal and seasonal variations of Hg0 air–surface exchange processes. Measurements of RGM deposition are limited and are known to have large uncertainties. Nevertheless, all of the measurements suggest that RGM can deposit very quickly onto any type of surface, with its Vd ranging from 0.5 to 6 cm s?1. The very limited data for Hgp suggest that its Vd values are in the range of 0.02–2 cm s?1.A resistance approach is commonly used in mercury transport models to estimate Vd for RGM and Hgp; however, there is a wide range of complexities in the dry deposition scheme of Hg0. Although resistance-approach based dry deposition schemes seem to be able to produce the typical Vd values for RGM and Hg0 over different surface types, more sophisticated air–surface exchange models have been developed to handle the bi-directional exchange processes. Both existing and newly developed dry deposition schemes need further evaluation using field measurements and intercomparisons within different modelling frameworks.  相似文献   

8.
Abstract

Bench-scale testing of elemental mercury (Hg0) sorption on selected activated carbon sorbents was conducted to develop a better understanding of the interaction among the sorbent, flue gas constituents, and Hg0. The results of the fixed-bed testing under simulated lignite combustion flue gas composition for activated carbons showed some initial breakthrough followed by increased mercury (Hg) capture for up to ~4.8 hr. After breakthrough, the Hg in the effluent stream was primarily in an oxidized form (>90%). Aliquots of selected activated carbons were exposed to simulated flue gas containing Hg0 vapor for varying time intervals to explore surface chemistry changes as the initial breakthrough, Hg capture, and oxidation occurred. The samples were analyzed by X-ray photoelectron spectroscopy to determine changes in the abundance and forms of sulfur, chlorine, oxygen, and nitrogen moieties as a result of interactions of flue gas components on the activated carbon surface during the sorption process. The data are best explained by a competition between the bound hydrogen chloride (HCl) and increasing sulfur [S(VI)] for a basic carbon binding site. Because loss of HCl is also coincident with Hg breakthrough or loss of the divalent Hg ion (Hg2+), the competition of Hg2+ with S(VI) on the basic carbon site is also implied. Thus, the role of the acid gases in Hg capture and release can be explained.  相似文献   

9.
Concentrations of different species of mercury in arctic air and precipitation have been measured at Ny-Ålesund (Svalbard) and Pallas (Finland) during 1996–1997. Typical concentrations for vapour phase mercury measured at the two stations were in the range of 0.7–2 ng m−3 whereas particulate mercury concentrations were below 5 pg m−3. Total mercury in precipitation was in the range 3–30 ng l−1. In order to evaluate the transport and deposition of mercury to the arctic from European anthropogenic sources, the Eulerian transport model HMET has been modified and extended to also include mercury species. A scheme for chemical conversion of elemental mercury to other species of mercury and deposition characteristics of different mercury species have been included in the model. European emission inventories for three different forms of Hg (Hg0, HgCl2 and Hgp) have been implemented in the numerical grid system for the HMET model.  相似文献   

10.
Abstract

Selective catalytic reduction (SCR) technology increasingly is being applied for controlling emissions of nitrogen oxides (NOx) from coal-fired boilers. Some recent field and pilot studies suggest that the operation of SCR could affect the chemical form of mercury (Hg) in coal combustion flue gases. The speciation of Hg is an important factor influencing the control and environmental fate of Hg emissions from coal combustion. The vanadium and titanium oxides, used commonly in the vanadia-titania SCR catalyst for catalytic NOx reduction, promote the formation of oxidized mercury (Hg2+).

The work reported in this paper focuses on the impact of SCR on elemental mercury (Hg0) oxidation. Bench-scale experiments were conducted to investigate Hg0 oxidation in the presence of simulated coal combustion flue gases and under SCR reaction conditions. Flue gas mixtures with different concentrations of hydrogen chloride (HCl) and sulfur dioxide (SO2) for simulating the combustion of bituminous coals and subbituminous coals were tested in these experiments. The effects of HCl and SO2 in the flue gases on Hg0 oxidation under SCR reaction conditions were studied. It was observed that HCl is the most critical flue gas component that causes conversion of Hg0 to Hg2+ under SCR reaction conditions. The importance of HCl for Hg0 oxidation found in the present study provides the scientific basis for the apparent coal-type dependence observed for Hg0 oxidation occurring across the SCR reactors in the field.  相似文献   

11.
Atmospheric concentrations of major reactive nitrogen (Nr) species were quantified using passive samplers, denuders, and particulate samplers at Dongbeiwang and Quzhou, North China Plain (NCP) in a two-year study. Average concentrations of NH3, NO2, HNO3, pNH4+ and pNO3 were 12.0, 12.9, 0.6, 10.3, and 4.7 μg N m−3 across the two sites, showing different seasonal patterns of these Nr species. For example, the highest NH3 concentration occurred in summer while NO2 concentrations were greater in winter, both of which reflected impacts of N fertilization (summer) and coal-fueled home heating (winter). Based on measured Nr concentrations and their deposition velocities taken from the literature, annual N dry deposition was up to 55 kg N ha−1. Such high concentrations and deposition rates of Nr species in the NCP indicate very serious air pollution from anthropogenic sources and significant atmospheric N input to crops.  相似文献   

12.
Experiments were performed to investigate the effect of ozone (O3) on mercury (Hg) emission from a variety of Hg-bearing substrates. Substrates with Hg(II) as the dominant Hg phase exhibited a 1.7 to 51-fold increase in elemental Hg (Hgo) flux and a 1.3 to 8.6-fold increase in reactive gaseous mercury (RGM) flux in the presence of O3-enriched clean (50 ppb O3; 8 substrates) and ambient air (up to ∼70 ppb O3; 6 substrates), relative to clean air (oxidant and Hg free air). In contrast, Hgo fluxes from two artificially Hgo-amended substrates decreased by more than 75% during exposure to O3-enriched clean air relative to clean air. Reactive gaseous mercury emissions from Hgo-amended substrates increased immediately after exposure to O3 but then decreased rapidly. These experimental results demonstrate that O3 is very important in controlling Hg emissions from substrates. The chemical mechanisms that produced these trends are not known but potentially involve heterogenous reactions between O3, the substrate, and Hg. Our experiments suggest they are not homogenous gas-phase reactions. Comparison of the influence of O3 versus light on increasing Hgo emissions from dry Hg(II)-bearing substrates demonstrated that they have a similar amount of influence although O3 appeared to be slightly more dominant. Experiments using water-saturated substrates showed that the presence of high-substrate moisture content minimizes reactions between atmospheric O3 and substrate-bound Hg. Using conservative calculations developed in this paper, we conclude that because O3 concentrations have roughly doubled in the last 100 years, this could have increased Hgo emissions from terrestrial substrates by 65–72%.  相似文献   

13.
Si L  Ariya PA 《Chemosphere》2011,84(8):1079-1084
Mercury is a global environmental contaminant with severe toxicity impact. The chemical processes resulting in the transformation of oxidized mercury species (Hg2+) to elemental mercury (Hg0), greatly affects the fate and transport of mercury in the natural environment. We hereby provide the first study on the photochemistry of Hg2+ with selected alkanethiols (R-SH) as model compounds to represent thiols and thiol-type binding sites on humic substances in natural waters because of the common sulfhydryl functional group (-SH). Kinetic studies were performed using cold vapor atomic fluorescence spectroscopy (CVAFS), the formation of Hg2+-thiol complexes (Hg(SR)2) were confirmed by UV-visible spectrometry and Atmospheric Pressure Chemical Ionization-Mass Spectrometry (APCI-MS), and the reaction products were analyzed using Electron Impact-Mass Spectrometry (EI-MS) and Solid Phase Microextraction coupled with Gas Chromatography-Mass Spectrometry (SPME/GC-MS). Our results indicated that the photoreduction of Hg2+ by selected alkanethiols may be mediated by Hg2+-thiol complexes to produce Hg0. Under our experimental conditions, the apparent first order rate constants obtained for 1-propanethiol, 1-butanethiol, and 1-pentanethiol were (2.0 ± 0.2) × 10−7 s−1, (1.4 ± 0.1) × 10−7 s−1, (8.3 ± 0.5) × 10−8 s−1, respectively. The effects of ionic strength, dissolved oxygen or chloride ion on reaction rates were found to be minimal under our experimental conditions. The identified products of the reaction between oxidized mercury species with selected alkanethiols (C3-C5) were Hg0 and disulfides (RS-SR). The potential environmental implications are herein discussed.  相似文献   

14.
Critical Limits for Hg(II) in soils, derived from chronic toxicity data   总被引:1,自引:0,他引:1  
Published chronic toxicity data for Hg(II) added to soils were assembled and evaluated to produce a data set comprising 52 chronic end-points, five each for plants and invertebrates and 42 for microbes. With end-points expressed in terms of added soil Hg(II) contents, Critical Limits were derived from the 5th percentiles of species sensitivity distributions, values of 0.13 μg (g soil)−1 and 3.3 μg (g soil organic matter)−1 being obtained. The latter value exceeds the currently recommended Critical Limit, used to determine Hg(II) Critical Loads in Europe, of 0.5 μg (g soil organic matter)−1. We also applied the WHAM/Model VI chemical speciation model to estimate concentrations of Hg2+ in soil solution, and derived an approximate Critical Limit Function (CLF) that includes pH; log [Hg2+]crit = −2.15 pH −17.10. Because they take soil properties into account, the soil organic matter-based limit and the CLF provide the best assessment of toxic threat for different soils. For differing representative soils, each predicts a range of up to 100-fold in the dry weight-based content of mercury that corresponds to the Critical Limit.  相似文献   

15.
Mercury pollution is caused by artisanal and small-scale gold mining (ASGM) operations along the Cikaniki River (West Java, Indonesia). The atmosphere is one of the primary media through which mercury can disperse. In this study, atmospheric mercury levels are estimated using the native epiphytic fern Asplenium nidus complex (A. nidus) as a biomonitor; these estimates shed light on the atmospheric dispersion of mercury released during mining.Samples were collected from 8 sites along the Cikaniki Basin during September-November, 2008 and September-November, 2009.The A. nidus fronds that were attached to tree trunks 1-3 m above the ground were collected and measured for total mercury concentration using cold vapor atomic absorption spectrometry (CVAAS) after acid-digestion. The atmospheric mercury was collected using porous gold collectors, and the concentrations were determined using double-amalgam CVAAS.The highest atmospheric mercury concentration, 1.8 × 103 ± 1.6 × 103 ng m−3, was observed at the mining hot spot, and the lowest concentration of mercury, 5.6 ± 2.0 ng m−3, was observed at the remote site from the Cikaniki River in 2009. The mercury concentrations in A. nidus were higher at the mining village (5.4 × 103 ± 1.6 × 103 ng g−1) than at the remote site (70 ± 30 ng g−1). The distribution of mercury in A. nidus was similar to that in the atmosphere; a significant correlation was observed between the mercury concentrations in the air and in A. nidus (r = 0.895, P < 0.001, n = 14). The mercury levels in the atmosphere can be estimated from the mercury concentration in A. nidus using a regression equation: log (HgA.nidu/ng g−1) = 0.740 log (HgAir/ng m−3) − 1.324.  相似文献   

16.
Stream water samples were collected over a range of hydrologic and seasonal conditions at three forested watersheds in the northeastern USA. Samples were analyzed for dissolved total mercury (THgd), DOC concentration and DOC composition, and UV254 absorbance across the three sites over different seasons and flow conditions. Pooling data from all sites, we found a strong positive correlation of THgd to DOC (r2 = 0.87), but progressively stronger correlations of THgd with the hydrophobic acid fraction (HPOA) of DOC (r2 = 0.91) and with UV254 absorbance (r2 = 0.92). The strength of the UV254 absorbance-THgd relationship suggests that optical properties associated with dissolved organic matter may be excellent proxies for THgd concentration in these streams. Ease of sample collection and analysis, the potential application of in-situ optical sensors, and the possibility for intensive monitoring over the hydrograph make this an effective, inexpensive approach to estimate THgd flux in drainage waters.  相似文献   

17.
Anthropogenic mercury emissions in China   总被引:18,自引:0,他引:18  
An inventory of mercury emissions from anthropogenic activities in China is compiled for the year 1999 from official statistical data. We estimate that China's emissions were 536 (±236) t of total mercury. This value includes open biomass burning, but does not include natural sources or re-emission of previously deposited mercury. Approximately 45% of the Hg comes from non-ferrous metals smelting, 38% from coal combustion, and 17% from miscellaneous activities, of which battery and fluorescent lamp production and cement production are the largest. Emissions are heaviest in Liaoning and Guangdong Provinces, where extensive smelting occurs, and in Guizhou Province, where there is much small-scale combustion of high-Hg coal without emission control devices. Emissions are gridded at 30×30 min spatial resolution. We estimate that 56% of the Hg in China is released as Hg0, 32% as Hg2+, and 12% as Hgp. Particulate mercury emissions are high in China due to heavy burning of coal in residential and small industrial settings without PM controls. Emissions of Hg2+ from coal-fired power plants are high due to the absence of flue-gas desulfurization units, which tend to dissolve the soluble divalent mercury. Metals smelting operations favor the production of elemental mercury. Much of the Hg is released from small-scale activities in rather remote areas, and therefore the activity levels are quite uncertain. Also, emissions test data for Chinese sources are lacking, causing uncertainties in Hg emission factors and removal efficiencies. Overall, we calculate an uncertainty level of ±44% (95% confidence interval) in the estimate of total emissions. We recommend field testing of coal combustors and smelters in China to improve the accuracy of these estimates.  相似文献   

18.
In the present study, we aim to investigate the extent of soil contamination by Hg, particularly by anthropogenic Hg, and tentatively estimate the total Hg (HgT) accumulation in topsoils (0-15 cm) in Fuyang, Zhejiang Province—a secondary Cu smelter of China. The results show that the levels of soil Hg in the vicinity of the smelters have been substantially elevated following local smelting activities. The spatial distribution of soil Hg in this area reveals a rapid decrease as the distance from the smelter reaches 1.5 km, which is probably due to the quick deposition process of particulate Hg and reactive gaseous Hg emitted from the smelters. The total accumulation of HgT in the topsoils of the study area of 10.9 km2 is approximately 365-561 kg and of which 346-543 kg might be contributed by anthropogenic emission alone with an annual emission of 17.3-27.2 kg Hg to the topsoils.  相似文献   

19.
Atmospheric mercury (Hg) species, including gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate-bound mercury (Hgp), were monitored near three sites, including a cement plant (monitored in 2007 and 2008), an urban site and a rural site (both monitored in 2005 and 2008). Although the cement plant was a significant source of Hg emissions (for 2008, GEM: 2.20 ± 1.39 ng m?3, RGM: 25.2 ± 52.8 pg m?3, Hgp 80.8 ± 283 pg m?3), average GEM levels and daytime average dry depositional RGM flux were highest at the rural site, when all three sites were monitored sequentially in 2008 (rural site, GEM: 2.37 ± 1.26 ng m?3, daytime RGM flux: 29 ± 40 ng m?2 day?1). Photochemical conversion of GEM was not the primary RGM source, as highest net RGM gains (75.9 pg m?3, 99.0 pg m?3, 149 m?3) occurred within 3.0–5.3 h, while the theoretical time required was 14–23 h. Instead, simultaneous peaks in RGM, Hgp, ozone (O3), nitrogen oxides, and sulfur dioxide in the late afternoon suggested short-range transport of RGM from the urban center to the rural site. The rural site was located more inland, where the average water vapor mixing ratio was lower compared to the other two sites (in 2008, rural: 5.6 ± 1.4 g kg?1, urban: 9.0 ± 1.1 g kg?1, cement plant: 8.3 ± 2.2 g kg?1). Together, these findings suggested short-range transport of O3 from an urban area contributed to higher RGM deposition at the rural site, while drier conditions helped sustain elevated RGM levels. Results suggested less urbanized environments may be equally or perhaps more impacted by industrial atmospheric Hg emissions, compared to the urban areas from where Hg emissions originated.  相似文献   

20.
Abstract

Waste distribution and compaction at the working face of municipal waste landfills releases mercury vapor (Hg0) to the atmosphere, as does the flaring of landfill gas. Waste storage and processing before its addition to the landfill also has the potential to release Hg0 to the air if it is initially present or formed by chemical reduction of HgII to Hg0 within collected waste. We measured the release of Hg vapor to the atmosphere during dumpster and transfer station activities and waste storage before landfilling at a municipal landfill operation in central Florida. We also quantified the potential contribution of specific Hg-bearing wastes, including mercury (Hg) thermometers and fluorescent bulbs, and searched for primary Hg sources in sorted wastes at three different landfills. Surprisingly large fluxes were estimated for Hg losses at transfer facilities (~100 mg/hr) and from dumpsters in the field (~30 mg/hr for 1,000 dumpsters), suggesting that Hg emissions occurring before landfilling may constitute a significant fraction of the total emission from the disposal/landfill cycle and a need for more measurements on these sources. Reducing conditions of landfill burial were obviously not needed to generate strong Hg0 signals, indicating that much of the Hg was already present in a metallic (Hg0) form. Attempts to identify specific Hg sources in excavated and sorted waste indicated few readily identifiable sources; because of effective mixing and diffusion of Hg0, the entire waste mass acts as a source. Broken fluorescent bulbs and thermometers in dumpsters emitted Hg0 at 10 to >100 μg/hr and continued to act as near constant sources for several days.  相似文献   

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