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1.
ABSTRACT

A case study was conducted to evaluate the SO2 emission reduction in a power plant in Central Mexico, as a result of the shifting of fuel oil to natural gas. Emissions of criteria pollutants, greenhouse gases, organic and inorganic toxics were estimated based on a 2010 report of hourly fuel oil consumption at the “Francisco Pérez Ríos” power plant in Tula, Mexico. For SO2, the dispersion of these emissions was assessed with the CALPUFF dispersion model. Emissions reductions of > 99% for SO2, PM and Pb, as well as reductions >50% for organic and inorganic toxics were observed when simulating the use of natural gas. Maximum annual (993 µg/m3) and monthly average SO2 concentrations were simulated during the cold-dry period (152–1063 µg/m3), and warm-dry period (239–432 µg/m3). Dispersion model results and those from Mexico City’s air quality forecasting system showed that SO2 emissions from the power plant affect the north of Mexico City in the cold-dry period. The evaluation of model estimates with 24 hr SO2 measured concentrations at Tepeji del Rio suggests that the combination of observations and dispersion models are useful in assessing the reduction of SO2 emissions due to shifting in fuels. Being SO2 a major precursor of acid rain, high transported sulfate concentrations are of concern and low pH values have been reported in the south of Mexico City, indicating that secondary SO2 products emitted in the power plant can be transported to Mexico City under specific atmospheric conditions.

Implications: Although the surroundings of a power plant located north of Mexico City receives most of the direct SO2 impact from fuel oil emissions, the plume is dispersed and advected to the Mexico City metropolitan area, where its secondary products may cause acid rain. The use of cleaner fuels may assure significant SO2 reductions in the plant emissions and consequent acid rain presence in nearby populated cities and should be compulsory in critical areas to comply with annual emission limits and health standards.  相似文献   

2.
The waste seawater discharged in coastal areas from coal-fired power plants equipped with a seawater desulfurization system might carry pollutants such as mercury from the flue gas into the adjacent seas. However, only very limited impact studies have been carried out. Taking a typical plant in Xiamen as an example, the present study targeted the distribution and sea–air transfer flux of volatile mercury in seawater, in order to trace the fate of the discharged mercury other than into the sediments. Samples from 28 sampling sites were collected in the sea area around two discharge outlets of the plant, daily and seasonally. Total mercury, dissolved gaseous mercury and dissolved total mercury in the seawater, as well as gaseous elemental mercury above the sea surface, were investigated. Mean concentrations of dissolved gaseous mercury and gaseous elemental mercury in the area were 183 and 4.48 ng m?3 in summer and 116 and 3.92 ng m?3 in winter, which were significantly higher than those at a reference site. Based on the flux calculation, the transfer of volatile mercury was from the sea surface into the atmosphere, and more than 4.4 kg mercury, accounting for at least 2.2 % of the total discharge amount of the coal-fired power plant in the sampling area (1 km2), was emitted to the air annually. This study strongly suggested that besides being deposited into the sediment and diluted with seawater, emission into the atmosphere was an important fate for the mercury from the waste seawater from coal-fired power plants.  相似文献   

3.
ABSTRACT

The main goal of this study was to evaluate the magnitude of outdoor exposure to fine particulate matter (PM10) potentially experienced by the population of metropolitan Mexico City. With the use of a geographic information system (GIS), spatially resolved PM10 distributions were generated and linked to the local population. The PM10 concentration exceeded the 24-hr air quality standard of 150 μg/m3 on 16% of the days, and the annual air quality standard of 50 μg/m3 was exceeded by almost twice its value in some places. The basic methodology described in this paper integrates spatial demographic and air quality databases, allowing the evaluation of various air pollution reduction scenarios. Achieving the annual air quality standard would represent a reduction in the annual arithmetic average concentration of 14 μg/m3 for the typical inhabitant. Human exposure to particulate matter (PM) has been associated with mortality and morbidity in Mexico City; reducing the concentration levels of this pollutant would represent a reduction in mortality and morbidity and the associated cost of such impacts. This methodology is critical to assessing the potential benefits of the current initiative to improve air quality implemented by the Environmental Metropolitan Commission of Mexico City.  相似文献   

4.
In this investigation, the concentrations of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particulate bound mercury (PBM) in ambient air were measured at the Hung Kuang (traffic) sampling site during September 27 to October 6, 2014. An ambient air mercury collection system (AAMCS) was utilized to measure simultaneously PBM, GEM, and RGM concentrations in ambient air. The results thus obtained demonstrate that the mean concentrations of PBM, GEM, and RGM were 38.57 ± 11.4 (pg/m3), 17.67 ± 5.56 (ng/m3) and 10.78 ± 2.8 (pg/m3), respectively, at this traffic-sampling site. The mean GEM/PBM and GEM/RGM concentration ratios were 458 and 1639, respectively. The results obtained herein demonstrate that AAMCS can be utilized to collect three phases of mercury simultaneously. The mean PBM, GEM, and RGM concentrations herein were compared with others found in Asia, America, Europe and Antarctica. The mean PBM, GEM, and RGM concentrations were found to be lowest in Asia and Antarctica. The mean PBM concentration in Europe was approximately eight times that in this investigation. The mean GEM and RGM concentrations in this study were 1.21 and 170 times those found in the United States.  相似文献   

5.
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   

6.
Measurements of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM), and particulate mercury (PHg) have been conducted at Lulin Atmospheric Background Station (LABS) in Taiwan since April 2006. This was the first long-term free tropospheric atmospheric Hg monitoring program in the downwind region of East Asia, which is a major Hg emission source region. Between April 13, 2006 and December 31, 2007, the mean concentrations of GEM, RGM, and PHg were 1.73 ng m?3, 12.1 pg m?3, and 2.3 pg m?3, respectively. A diurnal pattern was observed for GEM with afternoon peaks and nighttime lows, whereas the diurnal pattern of RGM was opposite to that of GEM. Spikes of RGM were frequently observed between midnight and early morning with concurrent decreases in GEM and relative humidity and increases in O3, suggesting the oxidation of GEM and formation of RGM in free troposphere (FT). Upslope movement of boundary layer (BL) air in daytime and subsidence of FT air at night resulted in these diurnal patterns. Considering only the nighttime data, which were more representative of FT air, the composite monthly mean GEM concentrations ranged between 1.06 and 2.06 ng m?3. Seasonal variation in nighttime GEM was evident, with lower concentrations usually occurring in summer when clean marine air masses prevailed. Between fall and spring, air masses passed the East Asian continent prior to reaching LABS, contributing to the elevated GEM concentrations. Analysis of GEM/CO correlation tends to support the argument. Good GEM/CO correlations were observed in fall, winter, and spring, suggesting influence of anthropogenic emission sources. Our results demonstrate the significance of East Asian Hg emissions, including both anthropogenic and biomass burning emissions, and their long-range transport in the FT. Because of the pronounced seasonal monsoon activity and the seasonal variation in regional wind field, export of the Asian Hg emissions to Taiwan occurs mainly during fall, winter, and spring.  相似文献   

7.
Regulatory control of mercury emission from anthropogenic sources has become a global concern in the recent past. Coal-fired power plants are one of the largest sources of anthropogenic mercury emission into the atmosphere. This paper summarizes the current reducing trend of mercury emission as co-beneficial effect by more stringent regulation changes to control primary air pollutants with introducing test results from the commercial coal-fired facilities and suggesting a guideline for future regulatory development in Korea. On average, mercury emission concentrations ranged 16.3–2.7 μg Sm?3, 2.4–1.1 μg Sm?3, 3.1–0.7 μg Sm?3 from anthracite coal-fired power plants equipped with electrostatic precipitator (ESP), bituminous coal-fired power plants with ESP + flue gas desulphurization (FGD) and bituminous coal-fired power plants with selective catalytic reactor (SCR) + cold side (CS) ? ESP + wet FGD, respectively. Among the existing air pollution control devices, the best configuration for mercury removal in coal-fired power plants was SCR + CS ? ESP + wet FGD, which were installed due to the stringent regulation changes to control primary air pollutants emission such as SO2, NOx and dust. It was estimated that uncontrolled and controlled mercury emission from coal-fired power plants as 10.3 ton yr?1 and 3.2 ton yr?1 respectively. After the installation of ESP, FGD and SCR system, following the enforcement of the stringent regulation, 7.1 ton yr?1 of mercury emission has been reduced (nearly 69%) from coal-fired power plants as a co-benefit control. Based on the overall study, a sample guideline including emission limits were suggested which will be applied to develop a countermeasure for controlling mercury emission from coal-fired power plants.  相似文献   

8.
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   

9.
From February 29 until June 15 2008 gaseous elemental mercury (GEM) fluxes above a snow covered surface was measured in Ny-Ålesund, Svalbard using a GEM flux gradient method. A clear seasonal pattern in the meteorological variables associated with the GEM flux was observed. For the first time in Ny-Ålesund a net deposition of GEM was recorded during polar night, despite the lack of Atmospheric Mercury Depletion Events (AMDE). 7500 ng m−2 GEM was emitted from the surface snow to the air during the entire study. The depositions of GEM and reactive gaseous mercury (RGM) were calculated to be 1500 and 1000 ng m−2, respectively, during the same time period. The GEM fluxes reported in this study were found to be comparable to GEM fluxes measured at other Arctic locations (i.e. Alert and Barrow), suggesting that GEM acts in a similar way throughout the Arctic. An assessment of the GEM flux gradient method used discovered a non-linear GEM concentration profile. The nonlinearity was explained by a non-stationary turbulence regime. The GEM flux calculated was not found to be representative for the entire surface boundary layer.  相似文献   

10.
Measurements of gaseous elemental mercury (GEM), particulate mercury (Hgp), and reactive gaseous mercury (RGM) were concurrently recorded at an urban site in Detroit and a rural site in Dexter, both in Michigan for the calendar year 2004. Their average concentrations (±standard deviation) for the urban area were 2.5 ± 1.4 ng m?3, 18.1 ± 61.0 pg m?3, and 15.5 ± 54.9 pg m?3, respectively, while their rural counterparts were 1.6 ± 0.6 ng m?3, 6.1 ± 5.5 pg m?3, and 3.8 ± 6.6 pg m?3, respectively. The medians of urban-to-rural ratios of Hg concentrations indicate approximately 1-fold, 2-fold, and 3-fold gradients between Detroit and Dexter for GEM, Hgp, and RGM, respectively. The urban–rural differences in Hg also varied considerably on different temporal scales and with wind flow patterns, which was most evident in RGM. Our results show that while Hg at both sites was impacted by regional sources, meteorological conditions, and photochemical transformations, the extent of variations in the observed urban-to-rural gradients, particularly in RGM, cannot be fully accounted for by these processes. Both analyses of the annual data and case studies indicate that the more variable and episodic nature of Hg, particularly RGM, seen in Detroit compared with Dexter, was the result of direct impact from local anthropogenic sources.  相似文献   

11.
Abstract

An entrained-flow system has been designed and constructed to simulate in-flight mercury (Hg) capture by sorbent injection in ducts of coal-fired utility plants. The test conditions of 1.2-sec residence time, 140 °C gas temperature, 6.7 m/sec (22 ft/sec) gas velocity, and 0–0.24 g/m3 (0–15 lbs of sorbent per 1 million actual cubic feet of flue gas [lb/MMacf]) sorbent injection rates were chosen to simulate conditions in the ducts. Four kinds of sorbents were used in this study. Darco Hg-LH served as a benchmark sorbent with which Hg control capability of other sorbents could be compared. Also, Darco-FGD was used as a representative raw activated carbon sorbent. Two different copper chloride-impregnated sorbents were developed in our laboratory and tested in the entrained-flow system to examine the possibility of using these sorbents at coal-fired power plants. The test results showed that one of the copper chloride sorbents has remarkable elemental mercury (Hg0) oxidation capability, and the other sorbent demonstrated a better performance in Hg removal than Darco Hg-LH.  相似文献   

12.
Semi-continuous measurements of ambient mercury (Hg) species were performed in Detroit, MI, USA for the calendar year 2003. The mean (±standard deviation) concentrations for gaseous elemental mercury (GEM), particulate mercury (HgP), and reactive gaseous mercury (RGM) were 2.2±1.3 ng m−3, 20.8±30.0, and 17.7±28.9 pg m−3, respectively. A clear seasonality in Hg speciation was observed with GEM and RGM concentrations significantly (p<0.001) greater in warm seasons, while HgP concentrations were greater in cold seasons. The three measured Hg species also exhibited clear diurnal trends which were particularly evident during the summer months. Higher RGM concentrations were observed during the day than at night. Hourly HgP and GEM concentrations exhibited a similar diurnal pattern with both being inversely correlated with RGM. Multivariate analysis coupled with conditional probability function analysis revealed the conditions associated with high Hg concentration episodes, and identified the inter-correlations between speciated Hg concentrations, three common urban air pollutants (sulfur dioxide, ozone, and nitric oxides), and meteorological parameters. This analysis suggests that both local and regional sources were major factors contributing to the observed temporal variations in Hg speciation. Boundary layer dynamics and the seasonal meteorological conditions, including temperature and moisture content, were also important factors affecting Hg variability.  相似文献   

13.
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m?2 h?1), emission in the summer (2.5 ng m?2 h?1), near zero flux in the fall (0.3 ng m?2 h?1), and emission in the winter (4.1 ng m?2 h?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.  相似文献   

14.
用于气态零价汞转化的催化剂研究   总被引:4,自引:0,他引:4  
零价汞的高效去除是燃煤烟气汞污染控制过程中的关键环节。为了促进烟气中的零价汞转化为易于去除的氧化态汞,分别考察了在有HCl存在时,几种过渡金属氧化物(Cu、Fe、Mn、Co和Zr)对零价汞氧化的催化作用,以筛选出性能较好的催化组分;为提高催化剂的抗SO2性能,分别尝试了利用几种金属元素(Sr、Ce、W和Mo)对催化剂进行掺杂改性的方法。结果表明,锰氧化物的催化作用最好,其最佳使用温度在573 K左右;SO2对零价汞的催化氧化有明显抑制作用,在无SO2及1 400 mg/m3SO2时锰催化剂对零价汞催化氧化效率分别为93%和78%。而Mo改性的锰氧化物催化剂的抗硫性能大幅提高,在1 400 mg/m3SO2存在的情况下其对零价汞的催化氧化效率可达到90%以上,较其他改性元素高。  相似文献   

15.
The number of gas turbine- (GT-) based power plants is rapidly increasing to meet the world’s power demands. Until a few years ago, fossil fuel, and specifically fuel oil, was considered the major energy source for gas turbine operation. Due to the high amount of pollution that fuel oil generates, natural gas has become a popular source of energy due to its lower emissions compared to fuel oil. As a result, many GTs have switched to natural gas as an alternative to fuel oil. However, pollutants expelled from GT-based power plants operating on natural gas impact surrounding air quality. The objective of this study was to examine the dispersion of nitrogen oxides (NOx) emitted from a GT-based power plant located in the Sultanate of Oman. Supported by CALPUFF dispersion modeling software, six scenarios were investigated in this study. The first four scenarios considered a case where the GT-based power plant was operating on natural gas during winter and summer and for open and combined cycle modes. The remaining two scenarios considered, for both open and combined cycle modes, the case where the GT-based power plant was operating on fuel oil. Whether run by natural gas or fuel oil, CALPUFF simulation results for both seasons showed that NOx concentrations were higher when GTs were used in the combined cycle mode. The concentrations were still lower than the allowable concentrations set by the United States Environmental Protection Agency (U.S. EPA) standards. In contrast, for the case where the power plant operated on fuel oil, the NOx one-hour average simulated results exceeded the allowable limits only when the combined cycle mode was activated.  相似文献   

16.
Gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) were measured on the University of Mississippi campus from July 2011 to June 2012. It is believed to be the first time that concentrations of atmospheric mercury species have been documented in northern Mississippi, and at a location with relatively large and sudden swings in population. The mean concentration (±1SD) of GEM was 1.54 ± 0.32 ng m−3; levels were lower and generally more stable during the winter (1.48 ± 0.22) and spring (1.46 ± 0.27) compared with the summer (1.56 ± 0.32) and fall (1.63 ± 0.42). Mean concentrations for GOM and PBM were 3.87 pg m−3 and 4.58 pg m−3, respectively; levels tended to be highest in the afternoon and lowest in the early morning hours. During the fall and spring academic semesters concentrations and variability of GOM and PBM both increased, possibly from vehicle exhaust. There were moderate negative correlations with wind speed (all species) and humidity (GOM and PBM). Backward air mass trajectory modeling for the ten highest peaks for each mercury species revealed that the majority of these events occurred from air masses that passed through the northern continental US region. Overall, this study illustrates the complexity of temporal fluctuations of airborne mercury species, even in a small town environment.  相似文献   

17.
As power production from renewable energy and natural gas grows, closures of some coal-fired power plants in Texas become increasingly likely. In this study, the potential effects of such closures on air quality and human health were analyzed by linking a regional photochemical model with a health impacts assessment tool. The impacts varied significantly across 13 of the state’s largest coal-fired power plants, sometimes by more than an order of magnitude, even after normalizing by generation. While some power plants had negligible impacts on concentrations at important monitors, average impacts up to 0.5 parts per billion (ppb) and 0.2 µg/m3 and maximum impacts up to 3.3 ppb and 0.9 µg/m3 were seen for ozone and fine particulate matter (PM2.5), respectively. Individual power plants impacted average visibility by up to 0.25 deciviews in Class I Areas. Health impacts arose mostly from PM2.5 and were an order of magnitude higher for plants that lack scrubbers for SO2. Rankings of health impacts were largely consistent across the base model results and two reduced form models. Carbon dioxide emissions were relatively uniform, ranging from 1.00 to 1.26 short tons/MWh, and can be monetized based on a social cost of carbon. Despite all of these unpaid externalities, estimated direct costs of each power plant exceeded wholesale power prices in 2016.

Implications: While their CO2 emission rates are fairly similar, sharply different NOx and SO2 emission rates and spatial factors cause coal-fired power plants to vary by an order of magnitude in their impacts on ozone, particulate matter, and associated health and visibility outcomes. On a monetized basis, the air pollution health impacts often exceed the value of the electricity generated and are of similar magnitude to climate impacts. This suggests that both air pollution and climate should be considered if externalities are used to inform decision making about power-plant dispatch and retirement.  相似文献   


18.
The physicochemical properties and the contamination levels of mercury and arsenic in roadway dust from Baoji, NW China were investigated using an Atomic Fluorescence Spectrophotometer. Contamination levels were assessed based on the geoaccumulation index and the enrichment factor. The results show that magnetic susceptibilities of roadway dust were higher than Holocene loess–soil of central Shaanxi Loess Plateau. The mean contents of organic matter, PM10 and PM100 were 8.8%, 21.8% and 98.6%, respectively. Mercury concentration ranged from 0.48 to 2.32 μg g?1, with a mean value of 1.11 μg g?1, 17.1 times the Chinese soil mercury background value and 37 times the Shaanxi soil mercury background value. Arsenic concentration ranged from 9.0 to 42.8 μg g?1, with a mean value of 19.8 μg g?1, 1.8 times the Chinese and Shaanxi soil arsenic background values. The geoaccumlation index and enrichment factor indicate that mercury in the dust mainly originated from anthropogenic sources with ratings of “strongly polluted” and “strongly to extremely polluted”, whereas arsenic in dust originated from both natural and anthropogenic sources, with a ratings of “moderately to strongly polluted” and “strongly polluted”. Industrial activities, such as a coal-fired power station, coke-oven plant, and cement manufacturing plant, augmented by vehicular traffic, are the anthropogenic sources of mercury and arsenic in the roadway dust.  相似文献   

19.
The study of mercury (Hg) cycle in Arctic regions is a major subject of concern due to the dramatic increases of Hg concentrations in ecosystem in the last few decades. The causes of such increases are still in debate, and an important way to improve our knowledge on the subject is to study the exchanges of Hg between atmosphere and snow during springtime. We organized an international study from 10 April to 10 May 2003 in Ny-Ålesund, Svalbard, in order to assess these fluxes through measurements and derived calculations.Snow-to-air emission fluxes of Hg were measured using the flux chamber technique between ∼0 and 50 ng m−2 h−1. A peak in Gaseous Elemental Mercury (GEM) emission flux from the snow to the atmosphere has been measured just few hours after an Atmospheric Mercury Depletion Event (AMDE) recorded on 22 April 2004. Surprisingly, this peak in GEM emitted after this AMDE did not correspond to any increase in Hg concentration in snow surface. A peak in GEM flux after an AMDE was observed only for this single event but not for the four other AMDEs recorded during this spring period.In the snow pack which is seasonal and about 40 cm depth above permafrost, Hg is involved in both production and incorporation processes. The incorporation was evaluated to ∼5–40 pg m2 h. Outside of AMDE periods, Hg flux from the snow surface to the atmosphere was the consequence of GEM production in the air of snow and was about ∼15–50 ng m−2 h−1, with a contribution of deeper snow layers evaluated to ∼0.3–6.5 ng m−2 h−1. The major part of GEM production is then mainly a surface phenomenon. The internal production of GEM was largely increasing when snow temperatures were close to melting, indicating a chemical process occurring in the quasi-liquid layer at the surface of snow grains.  相似文献   

20.
CALPUFF is an atmospheric source-receptor model recommended by the U.S. Environmental Protection Agency for use on a case-by-case basis in complex terrain and wind conditions. The ability of the model to provide useful information for exposure assessments in areas with those topographical and meteorological conditions has received little attention. This is an important knowledge gap for use of CALPUFF outside of regulatory applications, such as exposure analyses conducted in support of risk assessments and health studies. We compared deposition of cadmium (Cd), lead (Pb), and zinc (Zn) calculated with CALPUFF as a result of emissions from a zinc smelter with corresponding concentrations of the metals measured in attic dust and soil samples obtained from the surrounding area. On a point-by-point analysis, predictions from CALPUFF explained 11% (lead) to 53% (zinc) of the variability in concentrations measured in attic dust. Levels of heavy metals in soil interpolated to 100 residential addresses from the distribution of concentrations measured in soil samples also agreed well with deposition predicted with CALPUFF: R2 of 0.46, 0.76, and 079 for Pb, Cd, and Zn, respectively. Community-average concentrations of Cd, Pb, and Zn measured in soil were significantly (p < 0.0001) and strongly correlated (R2 ranged from 0.77 to 0.98) with predicted deposition rates. These findings demonstrate that CALPUFF can provide reasonably accurate predictions of the patterns of long-term air pollutant deposition in the near-field associated with emissions from a discrete source in complex terrain. Because deposition estimates are calculated as a linear function of air concentrations, CALPUFF is expected to be reliable model for prediction of long-term average, near-field ambient air concentrations in complex terrain as well.  相似文献   

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