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1.
This technical note describes a United States Environmental Protection Agency (U.S. EPA) measurement project to determine elemental mercury (Hg0) emissions from a mercury cell chlor-alkali (MCCA) facility in the southeastern U.S. during a 53-day monitoring campaign in the fall of 2006. The optical remote sensing (ORS) area source measurement method EPA OTM 10 was used to provide Hg0 flux data for the site. These results are reported and compared with cell room roof-vent monitoring data acquired by the facility for similar time periods. The 24-h extrapolated mercury emission rate estimates determined by the two monitoring approaches are shown to be similar with overall averages in the 400 g day?1 range with maximum values around 1200 g day?1. Results from the OTM 10 measurements, which include both cell room emissions and potential fugitive sources outside the cell room, are shown to be approximately 10% higher than cell room monitoring results indicating that fugitive emissions from outside the cell room produce a small but measurable effect for this site.  相似文献   

2.
In order to assess the importance of mercury emissions from naturally enriched sources relative to anthropogenic point sources, data must be collected that characterizes mercury emissions from representative areas and quantifies the influence of various environmental parameters that control emissions. With this information, we will be able to scale up natural source emissions to regional areas. In this study in situ mercury emission measurements were used, along with data from laboratory studies and statistical analysis, to scale up mercury emissions for the naturally enriched Ivanhoe Mining District, Nevada. Results from stepwise multi-variate regression analysis indicated that lithology, soil mercury concentration, and distance from the nearest fault were the most important factors controlling mercury flux. Field and lab experiments demonstrated that light and precipitation enhanced mercury emissions from alluvium with background mercury concentrations. Diel mercury emissions followed a Gaussian distribution. The Gaussian distribution was used to calculate an average daily emission for each lithologic unit, which were then used to calculate an average flux for the entire area of 17.1 ng Hg m−2 h−1. An annual emission of ∼8.7×104 g of mercury to the atmosphere was calculated for the 586 km2 area. The bulk of the Hg released into the atmosphere from the district (∼89%) is from naturally enriched non-point sources and ∼11% is emitted from areas of anthropogenic disturbance where mercury was mined. Mercury emissions from this area exceed the natural emission factor applied to mercury rich belts of the world (1.5 ng m−2 h−1) by an order of magnitude.  相似文献   

3.
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   

4.
Mercury (Hg) emissions from gasoline, diesel, and liquefied petroleum gas (LPG) vehicles were measured and speciated (particulate, oxidized, and elemental mercury). First, three different fuel types were analyzed for their original Hg contents; 571.1±4.5 ng L−1 for gasoline, 185.7±2.6 ng L−1 for diesel, and 1230.3±23.5 ng L−1 for LPG. All three vehicles were then tested at idling and driving modes. Hg in the exhaust gas was mostly in elemental form (Hg0), and no detectable levels of particulate (Hgp) or oxidized (Hg2+) mercury were measured. At idling modes, Hg concentrations in the exhaust gas of gasoline, diesel, and LPG vehicles were 1.5–9.1, 1.6–3.5, and 10.2–18.6 ng m−3, respectively. At driving modes, Hg concentrations were 3.8–16.8 ng m−3 (gasoline), 2.8–8.5 ng m−3 (diesel), and 20.0–26.9 ng m−3 (LPG). For all three vehicles, Hg concentrations at driving modes were higher than at idling modes. Furthermore, Hg emissions from LPG vehicle was highest of all three vehicle types tested, both at idling and driving modes, as expected from the fact that it had the highest original fuel Hg content.  相似文献   

5.
Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hgp) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g−1±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m−2 h−1(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m−2 h−1 and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m−2 h−1. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m−3), Hgp (3.0±6.2 pg m−3) and GEM (1.8±0.2 ng m−3) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hgp (25.8 pg m−3) and RGM (21.7 pg m−3) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hgp but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hgp at Maryhill.  相似文献   

6.
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   

7.
During the fall of 1998, the US Environmental Protection Agency and the Florida Department of Environmental Protection sponsored a 7-day study at the Ft. McHenry tunnel in Baltimore, MD with the objective of obtaining PM2.5 vehicle source profiles for use in atmospheric mercury source apportionment studies. PM2.5 emission profiles from gasoline and diesel powered vehicles were developed from analysis of trace elements, polycyclic aromatic hydrocarbons (PAH), and condensed aliphatic hydrocarbons. PM2.5 samples were collected using commercially available sampling systems and were extracted and analyzed using conventional well-established methods. Both inorganic and organic profiles were sufficiently unique to mathematically discriminate the contributions from each source type using a chemical mass balance source apportionment approach. However, only the organic source profiles provided unique PAH tracers (e.g., fluoranthene, pyrene, and chrysene) for diesel combustion that could be used to identify source contributions generated using multivariate statistical receptor modeling approaches. In addition, the study found significant emission of gaseous elemental mercury (Hg0), divalent reactive gaseous mercury (RGM), and particulate mercury (Hg(p)) from gasoline but not from diesel powered motor vehicles. Fuel analysis supported the tunnel measurement results showing that total mercury content in all grades of gasoline (284±108 ng L−1) was substantially higher than total mercury content in diesel fuel (62±37 ng L−1) collected contemporaneously at local Baltimore retailers.  相似文献   

8.
We compare a global model of mercury to sediment core records to constrain mercury emissions from the 19th century North American gold and silver mining. We use information on gold and silver production, the ratio of mercury lost to precious metal produced, and the fraction of mercury lost to the atmosphere to calculate an a priory mining inventory for the 1870s, when the historical gold rush was at its highest. The resulting global mining emissions are 1630 Mg yr?1, consistent with previously published studies. Using this a priori estimate, we find that our 1880 simulation over-predicts the mercury deposition enhancements archived in lake sediment records. Reducing the mining emissions to 820 Mg yr?1 improves agreement with observations, and leads to a 30% enhancement in global deposition in 1880 compared to the pre-industrial period. For North America, where 83% of the mining emissions are located, deposition increases by 60%. While our lower emissions of atmospheric mercury leads to a smaller impact of the North American gold rush on global mercury deposition than previously estimated, it also implies that a larger fraction of the mercury used in extracting precious metals could have been directly lost to local soils and watersheds.  相似文献   

9.
Most studies on the atmospheric behaviour of mercury in North America have excluded a detailed treatment of natural mercury emissions. The objective of this work is to report a detailed simulation of the atmospheric mercury in a domain that covers a significant part of North America and includes not only anthropogenic mercury emissions but also those from natural sources including vegetation, soil and water.The simulations were done using a natural mercury emission model coupled with the US EPA's SMOKE/CMAQ modelling system. The domain contained 132×90 grid cells at a resolution of 36 km, covering the continental United States, and major parts of Canada and Mexico. The simulation was carried out for 2002, using boundary conditions from a global mercury model. Estimated total natural mercury emission in the domain was 230 tonnes (1 tonne=1000 kg) and the ratio of natural to anthropogenic emissions varied from 0.7 in January to 3.2 in July. Average total gaseous mercury (TGM) concentration ranged between 1 and 4 ng m−3. Good agreement was found between the modelled results and measurements at three Ontario sites for ambient mercury concentrations, and at 72 mercury deposition network sites in the domain for wet deposition. The correlation coefficient between the simulated and the measured values of the daily average TGM at three monitoring sites varied between 0.48 and 0.64. When natural emissions were omitted, the correlation coefficients dropped to between 0.15 and 0.40. About 335 tonnes of mercury were deposited in the domain during the simulation period but overall, it acted as a net source of mercury and contributed about 21 tonnes to the global pool. The net deposition of mercury to the Great Lakes was estimated to be about 2.4 tonnes. The estimated deposition values were similar to those reported by other researchers.  相似文献   

10.
The Florida Everglades Dry-Deposition Study (FEDDS) was designed to test the viability of using new and existing measurement techniques in the estimation of the dry-depositional loading of speciated mercury (elemental gaseous, reactive gaseous and particulate) to a mixed sawgrass (Cladium jamaicense) and cattail (Typha domingensis) stand within the Florida Everglades. Measurement intensives were performed during 24 February–04 March 1999 and 05–21 June 2000, which corresponded to the climatological dry and wet seasons in South Florida, respectively. During these intensives, direct measurements of mercury dry-deposition were made using a newly developed surrogate water surface technique. These direct measurements were compared with modeled estimates of mercury dry-deposition to the site that were obtained through the use of an inferential or “bigleaf” model that was modified for use with speciated mercury. On-site measurements of ambient speciated mercury concentrations and numerous micrometeorological variables were used as input to the model.The average mercury dry-deposition measured during the 1999 FEDDS measurement intensive was 13.3±4.0 ng m−2 day−1, while the modeled deposition for this period was 3.4±2.3 ng m−2 day−1. The average mercury dry-deposition measured during the 2000 FEDDS measurement intensive was lower, 5.9±2.8 ng m−2 day−1, while the average modeled deposition for this period was 1.8±0.6 ng m−2 day−1. A least-squares linear regression suggests that the model was able to explain 74% and 73% of the variability in the datasets for the 1999 and 2000 FEDDS intensives, respectively. While reported reductions in total mercury emissions across South Florida between study periods could explain the reductions in both the measured and predicted mercury dry-deposition estimates, the increased presence of cumulus convection during the summer-intensive could have also resulted in a removal of reactive and particulate mercury species within the atmosphere of South Florida.  相似文献   

11.
There are inadequate measurements of surface ambient concentrations of mercury species and their deposition rates for the UK deposition budget to be characterized. In order to estimate the overall mercury flux budget for the UK, a simple long-term 1D Lagrangian trajectory model was constructed that treats emissions (1998), atmospheric transformation and deposition across Europe. The model was used to simulate surface concentrations of mercury and deposition across Europe at a resolution of 50 km×50 km and across the UK at 20 km×20 km. The model appeared to perform adequately when compared with the few available measurements, reproducing mean concentrations of elemental gaseous mercury at particular locations and the magnitude of regional gradients. The model showed that 68% of the UK's mercury emissions are exported and 32% deposited within the UK. Of deposition to the UK, 25% originates from the Northern Hemisphere/global background, 41% from UK sources and 33% from other European countries. The total mercury deposition to the UK is in good agreement with other modelling, 9.9 tonne yr−1 cf. 9.0 tonne yr−1, for 1998. However, the attribution differs greatly from the results of other coarser-scale modelling, which allocates 55% of the deposition to the UK from UK sources, 4% from other European countries and 60% from the global background atmosphere. The model was found to be sensitive to the speciation of emissions and the dry deposition velocity of elemental gaseous mercury. The uncertainties and deficiencies are discussed in terms of model parameterization and input data, and measurement data with which models can be validated. There is an urgent requirement for measurements of removal terms, concentrations, and deposition with which models can be parameterized and validated.  相似文献   

12.
Spatial distribution of SO2 emission inventory for 1994 from fuel combustion and industrial activities in Shanxi province, the Peoples’ Republic of China, has been created with 1/6°×1/4° latitude/longitude resolution. Total annual SO2 emissions in 1994 in the province were estimated to be 669 GgS, of which 180 GgS were emitted in winter, 170 GgS in spring, 156 GgS in summer, and 163 GgS in fall. For the first time this emission inventory includes SO2 emissions from village and township enterprises. Although SO2 emissions from major industries were under control, SO2 emissions from village and township enterprises became the major threat to the environment in the province.  相似文献   

13.
The present study presents the first detailed inventory for non-methane hydrocarbon emissions from vegetation over Greece. The emission inventory, based on a Geographic Information System (GIS), has a spatial resolution of 5×5 km2 and a time resolution of 1 h. For the area under study, the calculated yearly monoterpene emissions are higher than the corresponding isoprene ones. In addition to the methodology presented here, the CORINAIR methodology was also applied for the calculation of emission rates. This resulted in orders of magnitude differences in the calculated emission rates. The CORINAIR methodology is judged to lead to unrealistically high values of biogenic NMHC emission rates. The temperature dependence of the CORINAIR correction factors seems to affect most the emissions, together with grazing land emission factors.  相似文献   

14.
The composition of landfill gas (LFG) was analyzed for vapor-phase mercury (Hg) (primarily in its elemental form, Hg0) and relevant environmental parameters from 42 out of 106 ventpipes placed across two different sectors of the Nan-Ji-Do (NJD) landfill site in Seoul, Korea during September/October 2000. Results of our studies showed that large quantities of Hg emanated through these ventpipes which were infiltrated deep into the waste layer. The mean concentration of Hg, computed using the data sets collected from 42 ventpipes, was 420 ng m−3 with a range of 3.45–2952 ng m−3. Because large differences were apparent in its concentration levels not only between the two sectors of 1 and 2 but also between the plain and slope areas, evaluation of the data was made by dividing them into four different categories, namely plain areas of sectors 1 and 2 and slope areas of sectors 1 and 2. By categorizing the data in such a manner, the emission fluxes of ventilated Hg were estimated for each data group at the NJD site. The flux values of Hg for each data group were distinguished so that the enhanced fluxes were observed in plain compared to slope areas. The computed LFG fluxes of Hg from the whole NJD site were on the order of 23 g on an annual basis. The overall results of our study suggest that the vent emission of Hg from the study site is comparable in magnitude to those reported previously (e.g., the Florida landfill sites in US), while the LFG emissions of Hg may not necessarily be the most dominant source in the NJD site.  相似文献   

15.
The global atmospheric emissions of the 16 polycyclic aromatic hydrocarbons (PAHs) listed as the US EPA priority pollutants were estimated using reported emission activity and emission factor data for the reference year 2004. A database for emission factors was compiled, and their geometric means and frequency distributions applied for emission calculation and uncertainty analysis, respectively. The results for 37 countries were compared with other PAH emission inventories. It was estimated that the total global atmospheric emission of these 16 PAHs in 2004 was 520 giga grams per year (Gg y?1) with biofuel (56.7%), wildfire (17.0%) and consumer product usage (6.9%) as the major sources, and China (114 Gg y?1), India (90 Gg y?1) and United States (32 Gg y?1) were the top three countries with the highest PAH emissions. The PAH sources in the individual countries varied remarkably. For example, biofuel burning was the dominant PAH source in India, wildfire emissions were the dominant PAH source in Brazil, while consumer products were the major PAH emission source in the United States. In China, in addition to biomass combustion, coke ovens were a significant source of PAHs. Globally, benzo(a)pyrene accounted for 0.05% to 2.08% of the total PAH emission, with developing countries accounting for the higher percentages. The PAH emission density varied dramatically from 0.0013 kg km?2 y in the Falkland Islands to 360 kg km?2 y in Singapore with a global mean value of 3.98 kg km?2 y. The atmospheric emission of PAHs was positively correlated to the country's gross domestic product and negatively correlated with average income. Finally, a linear bivariate regression model was developed to explain the global PAH emission data.  相似文献   

16.
This paper gives the dust emission inventory in the Northern China where the climate is very dry and large desert areas exist. Before calculating the distribution of fugitive dust emission factors (emission rates of particles smaller than 0.05 mm in diameter) from natural surfaces with a US EPA formula, Chinese data of pedology and climatology were processed so as to suit requirements of the formula. The computed dust emission factors for this environment of Northern China are shown by contours, their distribution and seasonal variations are briefly discussed. The dust emission rate in the area increases from east to west by five orders. Also, the total amount of the dust emitted from natural surfaces of Northern China into the atmosphere is found to be some 43 million t yr-1, with half of the emissions concentrated in the spring season (March–May).  相似文献   

17.
Motor vehicle emissions of ammonia have been measured at a California highway tunnel in the San Francisco Bay area. Between 1999 and 2006, light-duty vehicle ammonia emissions decreased by 38 ± 6%, from 640 ± 40 to 400 ± 20 mg kg?1. High time resolution measurements of ammonia made in summer 2001 at the same location indicate a minimum in ammonia emissions correlated with slower-speed driving conditions. Variations in ammonia emission rates track changes in carbon monoxide more closely than changes in nitrogen oxides, especially during later evening hours when traffic speeds are highest. Analysis of remote sensing data of Burgard et al. (Environmental Science Technology 2006, 40, 7018–22) indicates relationships between ammonia and vehicle model year, nitrogen oxides, and carbon monoxide. Ammonia emission rates from diesel trucks were difficult to measure in the tunnel setting due to the large contribution to ammonia concentrations in a mixed-traffic bore that were assigned to light-duty vehicle emissions. Nevertheless, it is clear that heavy-duty diesel trucks are a minor source of ammonia emissions compared to light-duty gasoline vehicles.  相似文献   

18.
Size-fractionated particles were collected at two sites from July 2004 to April 2006 in Shanghai. The mercury in particles was extracted and divided operationally into four species: exchangeable particulate mercury (EXPM), HCl-soluble particulate mercury (HPM), elemental particulate mercury (EPM) and residual particulate mercury. The total particulate Hg concentration during the study period ranged from 0.07 ng m?3 to 1.45 ng m?3 with the average 0.56 ± 0.22 ng m?3 at site 1, while 0.20 ng m?3–0.47 ng m?3 with the average 0.33 ± 0.09 ng m?3 at site 2, which is far higher than some foreign cities and comparable to some cities with heavy air pollution in China. The Hg mass content also displayed evident size distribution, with higher value in PM1.6–3.7, somewhat higher or lower than the source profile. EXAM was only found in the summer, HPM have higher percentage in summer and fall rather than in winter and spring. The different mercury species showed different correlation to temperature, relative humidity, wind speed. HPM positively depends on temperature at both sites which implies the importance of mercury transformation on particles. In foggy days TPM increased greatly, but HPM didn't vary greatly as anticipated. Instead, RPM gained a distinguished increase. It demonstrated that aqueous reaction and complex heterogenic reactions in droplet might happen in acidic environment. The correlation of mercury with other pollutants including SO2, NO2, CO and PM10 varies with the different mercury forms. Hybrid single-particle lagrangian integrated trajectories (HYSPLIT) model was used to back trace air mass at different representative days and results indicated that transportation from Huabei Plain will increase mercury concentration in winter and fall to some extent. The possible existing compounds and their atmospheric behavior of HPM, EPM and RPM were calculated and the compared to analyze its implication on atmospheric mercury cycle.  相似文献   

19.
On the basis of the last inventory of forests and climatic conditions in Poland, a national evaluation of the emissions of reactive volatile organic compounds (VOCs) was carried out. Calculations took into account the composition and age structure of forests as well as the temperature dependencies of VOC emission rate for the main European forest-forming tree species. In the case of isoprene, the dependence on illumination level and day length was also taken into account. Estimations were made for all 49 administrative regions of Poland. Depending on weather conditions in different years, the total VOC emission of Polish forests can be in the range 186–763 kt yr−1. For instance, for a moderately warm year, 1992, it was estimated at 440.6 kt, which represents 25% of the total VOC emissions in Poland.  相似文献   

20.
A comprehensive, spatially resolved (0.25°×0.25°) fossil fuel consumption database and emissions inventory was constructed, for India, for the first time. Emissions of sulphur dioxide and aerosol chemical constituents were estimated for 1996–1997 and extrapolated to the Indian Ocean Experiment (INDOEX) study period (1998–1999). District level consumption of coal/lignite, petroleum and natural gas in power plants, industrial, transportation and domestic sectors was 9411 PJ, with major contributions from coal (54%) followed by diesel (18%). Emission factors for various pollutants were derived using India specific fuel characteristics and information on combustion/air pollution control technologies for the power and industrial sectors. Domestic and transportation emission factors, appropriate for Indian source characteristics, were compiled from literature. SO2 emissions from fossil fuel combustion for 1996–1997 were 4.0 Tg SO2 yr−1, with 756 large point sources (e.g. utilities, iron and steel, fertilisers, cement, refineries and petrochemicals and non-ferrous metals), accounting for 62%. PM2.5 emitted was 0.5 and 2.0 Tg yr−1 for the 100% and the 50% control scenario, respectively, applied to coal burning in the power and industrial sectors. Coal combustion was the major source of PM2.5 (92%) primarily consisting of fly ash, accounting for 98% of the “inorganic fraction” emissions (difference between PM2.5 and black carbon+organic matter) of 1.6 Tg yr−1. Black carbon emissions were estimated at 0.1 Tg yr−1, with 58% from diesel transport, and organic matter emissions at 0.3 Tg yr−1, with 48% from brick-kilns. Fossil fuel consumption and emissions peaked at the large point industrial sources and 22 cities, with elevated area fluxes in northern and western India. The spatial resolution of this inventory makes it suitable for regional-scale aerosol-climate studies. These results are compared to previous studies and differences discussed. Measurements of emission factors for Indian sources are needed to further refine these estimates.  相似文献   

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