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1.
Abstract

In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NOx) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NOx emissions reductions imposed on the utility sector by the NOx State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NOx emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NOx SIP Call. Comparison of the “no-control” with the “2002” scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NOx emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.  相似文献   

2.
The first observations of size-dependent cloud and fog drop inorganic ion and trace metal concentrations obtained using the Colorado State University 5-Stage cloud water collector (CSU 5-Stage) during field studies of orographic clouds (Whiteface Mountain, NY, July 1998) and radiation fogs (Davis, CA, January 1999) are reported. Although some mixing between drop sizes occurs, the CSU 5-Stage effectively separates the largest drops (>≈30 μm in diameter) from the smallest ones (<≈10 μm in diameter) permitting the discernment of size-dependent drop composition not possible with previous two- or three-stage collectors. At Whiteface, pH and the concentrations of the “major” ions −NH4+, NO3, and SO42−—appeared largely independent of drop size as measured by a two-stage collector. The same major ion concentrations differed in Davis fogs by up to a factor of approximately 10 in the two-stage collector with consistently higher small drop concentrations. In both locations, CSU 5-Stage data generally indicate a greater range of concentrations is present across the drop size spectrum. CSU 5-Stage data show “U”- shaped profiles of major ion concentration vs. drop size at Whiteface and “L”- shaped profiles at Davis and the maximum/minimum concentration differences between fractions increased up to a factor of 2 (Whiteface) and 30 (Davis). Lower concentration species at both locations showed multiple concentration vs. drop size profiles with CSU 5-Stage data again exhibiting more variability than observed with the two-stage collector. While rarely reported, significant nitrite concentrations—relatively higher in the larger drops—were observed, and copper concentrations merit further investigation in the Davis fogs. The findings presented here are consistent with other studies. The implications and benefits of the increased resolution of size-dependent drop composition provided by the CSU 5-Stage are explored for the Davis fogs in a companion paper (Moore et al., Atmos. Environ. (2004), this issue).  相似文献   

3.
ABSTRACT

During wintertime, haze episodes occur in the Dallas-Ft. Worth (DFW) urban area. Such episodes are characterized by substantial light scattering by particles and relatively low absorption, leading to so-called “white haze.” The objective of this work was to assess whether reductions in the emissions of SO2 from specific coal-fired power plants located over 100 km from DFW could lead to a discernible change in the DFW white haze. To that end, the transport, dispersion, deposition, and chemistry of the plume of a major power plant were simulated using a reactive plume model (ROME). The realism of the plume model simulations was tested by comparing model calculations of plume concentrations with aircraft data of SF6 tracer concentrations and ozone concentrations. A second-order closure dispersion algorithm was shown to perform better than a first-order closure algorithm and the empirical Pasquill-Gifford-Turner algorithm. For plume impact assessment, three actual scenarios were simulated, two with clear-sky conditions and one with the presence of fog prior to the haze. The largest amount of sulfate formation was obtained for the fog episode. Therefore, a hypothetical scenario was constructed using the meteorological conditions of the fog episode with input data values adjusted to be more conducive to sulfate formation. The results of the simulations suggest that reductions in the power plant emissions lead to less than proportional reductions in sulfate concentrations in DFW for the fog scenario. Calculations of the associated effects on light scattering using Mie theory suggest that reduction in total (plume + ambient) light extinction of less than 13% would be obtained with a 44% reduction in emissions of SO2 from the modeled power plant.  相似文献   

4.
Abstract

It is important to understand the effects of emission controls on concentrations of ozone, fine particulate matter (PM2.5), and hazardous air pollutants (HAPs) simultaneously, to evaluate the full range of health, ecosystem, and economic effects. Until recently, the capability to simultaneously evaluate interrelated atmospheric pollutants (“one atmosphere” analysis) was unavailable to air quality managers. In this work, we use an air quality model to examine the potential effect of three emission reductions on concentrations of ozone, PM2.5, and four important HAPs (formaldehyde, acetaldehyde, acrolein, and benzene) over a domain centered on Philadelphia for 12-day episodes in July and January 2001. Although NOx controls are predicted to benefit PM2.5 concentrations and sometimes benefit ozone, they have only a small effect on formaldehyde, slightly increase acetaldehyde and acrolein, and have no effect on benzene in the July episode. Concentrations of all pollutants except benzene increase slightly with NOx controls in the January simulation. Volatile organic compound controls alone are found to have a small effect on ozone and PM2.5, a less than linear effect on decreasing aldehydes, and an approximately linear effect on acrolein and benzene in summer, but a slightly larger than linear effect on aldehydes and acrolein in winter. These simulations indicate the difficulty in assessing how toxic air pollutants might respond to emission reductions aimed at decreasing criteria pollutants such as ozone and PM2.5.  相似文献   

5.
A new potential source of elevated chloroform (CHCl3) concentrations in urban air is reported. The exhaust gases from gasoline internal combustion engines operated on conventional “leaded” fuel and not equipped with catalytic converters contain parts-per-billion concentrations of chloroform which can, in congested urban areas, contribute significantly to the ambient concentration of chloroform. Exhaust gases from engines burning conventional “leaded” gasoline contain much higher levels of chloroform than do exhaust gases from engines equipped with catalytic converters and operating on “nonleaded” gasoline.  相似文献   

6.
We investigated a two-week episode with high PM concentrations in California Central Valley during the Christmas–New Year of 2000–2001 using a modeling system that consists of a computationally efficient, 3-D photochemical–microphysical transport model, a mesoscale meteorological model, emission models, and an evaluation package. One hundred simulations were conducted with fine resolutions and observational constraints, to reproduce spatial and temporal features of observed PM concentrations and to understand the formation mechanism of the episode. Simulated PM concentrations consist of secondary inorganic components, mainly ammonium nitrate, and total carbon in areas with elevated concentrations in the accumulation mode, and consist of mainly dust and sea salt in the coarse mode. Simulated oxidants and nitrate were significantly elevated over the valley, and the latter showed much less amplitude than the former. Simulated PM concentrations were evaluated with observations systematically with spatially and temporally paired method, a more restrictive multivariate method (NMFROC), and a more flexible “gradient evaluation” method. The paired evaluation shows that high correlation coefficient (R = ~0.8) and low fractional error (FE = ~0.1) could be achieved at stations with elevated 24-h concentration of PM in the accumulation mode in some simulations. The NMFROC method was used to extract useful information from seemingly failed simulations. A “gradient evaluation” method is introduced here to extract additional information from simulations. We found that emission reductions of NOx and AVOC showed similar effects on percentage basis in different areas, and both are more effective than reducing NH3 for abating elevated concentrations of accumulation mode PM in California Central Valley during the winter episode.  相似文献   

7.
A quantitative single-particle analytical technique, called low-Z particle electron probe X-ray microanalysis, combined with the utilization of their morphological information on individual particles, was applied to characterize six aerosol samples collected in one Korean city, Incheon, during March 9–15, 2006. The collected supermicron aerosol particles were classified based on their chemical species and morphology on a single-particle basis. Many different particle types were identified and their emission source, transport, and reactivity in the air were elucidated. In the samples, particles in the “soil-derived particles” group were the most abundant, followed by “reacted sea-salts”, “reacted CaCO3-containing particles”, “genuine sea-salts”, “reacted sea-salts + others”, “Fe-containing particles”, “anthropogenic organics”, (NH4)2SO4, “K-containing particles”, and “fly ash”. The application of this single-particle analysis, fully utilizing their chemical compositional and morphological data of individual particles, clearly revealed the different characteristics of the six aerosol samples. For samples S3 and S5, which were sampled during two Asian dust storm events, almost all particles were of soil origin that had not experienced chemical modification and that did not entrain sea-salts during their long-range transport. For sample S1, collected at an episodic period of high PM10 concentration and haze, anthropogenic, secondary, and soil-derived particles emitted from local sources were predominant. For samples S2, S4, and S6, which were collected on average spring days with respect to their PM10 concentrations, marine originated particles were the most abundant. Sample S2 seems to have been strongly influenced by emissions from the Yellow Sea and Korean peninsula, sample S4 had the minimum anthropogenic influence among the four samples collected in the absence of any Asian dust storm event, and sample S6 seems to have entrained air pollutants that had been transported from mainland China over the Yellow Sea to Korea.  相似文献   

8.
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   

9.
《Chemosphere》1997,34(2):345-355
The major inorganic components identified by ion-molecule reaction mass spectrometry (IMR-MS) raw gas measurements performed at the TAMARA facility include O2, H2O, CO2, HCl, SO2 and NO Higher concentrations of organic components, i.e. organic substance amounts > 10 m:1/m3 are not observed during normal operation. The concentrations of acetic and formic acids measured in the raw gas by the IMR-MS method range between “not detectable” (i.e. < 0.5 mg/Nm3) and 5 mg/Nm3. A relationship to the incineration parameters has not yet been established In case of operation failures, which are indicated by a CO increase, other organic compounds, e.g. acetaldehyde or benzene can be identified by the IMR-MS method Hence, the results obtained by IMR-MS in on-line emission control of a waste incineration gas are far more precise than the FID values. By IMR-MS measurements above the waste bed, a multitude of strong signals are recorded, which indicates the presence of a number of organic compounds in high concentrations (10 – 10000 mg/Nm3). A quantification during a “snapshot” has been accomplished for benzene (4000 mg/Nm3) and toluene (300 mg/Nm3).  相似文献   

10.
In this paper, the Gaussian Atmospheric Dispersion Modeling System (ADMS4) was coupled with field observations of surface meteorology and concentrations of several air quality indicators (nitrogen oxides (NOX), carbon monoxide (CO), fine particulate matter (PM10) and sulfur dioxide (SO2)) to test the applicability of source emission factors set by the European Environment Agency (EEA) and the United States Environmental Protection Agency (USEPA) at an industrial complex. Best emission factors and data groupings based on receptor location, type of terrain and wind speed, were relied upon to examine model performance using statistical analyses of simulated and observed data. The model performance was deemed satisfactory for several scenarios when receptors were located at downwind sites with index of agreement d values reaching 0.58, fractional bias “FB” and geometric mean bias “MG” values approaching 0 and 1, respectively, and normalized mean square error “NMSE” values as low as 2.17. However, median ratios of predicted to observed concentrations “Cp/Co” at variable downstream distances were 0.01, 0.36, 0.76 and 0.19 for NOX, CO, PM10 and SO2, respectively, and the fraction of predictions within a factor of two of observations “FAC2” values were lower than 0.5, indicating that the model could not adequately replicate all observed variations in emittant concentrations. Also, the model was found to be significantly sensitive to the input emission factor bringing into light the deficiency in regulatory compliance modeling which often uses internationally reported emission factors without testing their applicability.
Implications In the absence of site-specific source emission factors, the use of internationally reported emission factors without testing their validity may generate significant errors. Instead, recorded field measurements and meteorological data may be combined with atmospheric transport and dispersion models to better estimate source emissions, particularly in regulatory compliance studies. In this context, lower model performance is expected at higher wind speeds for most indicators such as CO, PM10, and SO2.  相似文献   

11.
Maps of the annual average of the NO2 concentration in an urban area are generally built from temporary seasonal measurements, as in 2001 at Mulhouse (France). To improve the precision of the estimation, auxiliary information about the environment can be used. Instead of kriging the average of the two seasonal measurements (in “winter” and in “summer”), cokriging these seasonal values guarantees the consistency of seasonal and annual estimations. Even more, cokriging allows the use of “incomplete series” at the sites measured during only one season. Based on cokriging, an optimization of the sampling is studied, while alternating the seasonal measurements on a part of the sites.Using the linear model of coregionalization, the fitting of simple and cross-variograms reveals a remarkable spatial decomposition of the seasonal concentrations. The different spatial components are interpreted in terms of physico-chemical processes of production, transformation or destruction of the NO2 in urban atmosphere.  相似文献   

12.
ABSTRACT

Three years of hourly averaged PM10 (particulate matter less than 10 Lrm in diameter) tapered element oscillating microbalance (TEOM) data from 10 sites in the large coastal valley incorporating Greater Vancouver were used to investigate the spatiotemporal dimensions and air pollution meteorology of particulate pollution. During the period studied, the provincial “acceptable” objective daily concentration of 50 μg m-3 was exceeded at 7 of the 10 sites. The highest annual, seasonal, and maximum hourly concentrations were recorded at Abbotsford in the central valley. Mean seasonal PM10 concentrations were highest in the wintertime in the western Lower Fraser Valley (LFV) and in the summertime at the central and eastern valley locations. Within the network, interstation correlations of daily average concentrations exceed 0.8 at interstation distances less than 20 km and decrease thereafter. For daily maximum concentrations (hourly), interstation correlations decrease sharply with distance. Meteorological conditions responsible for elevated par-ticulate concentrations in the LFV are associated with (1) short periods (1- to 3-hr duration) of reduced dispersion during summer nights at sites close to primary sources, (2) summer anticyclonic conditions when photochemical pollutant concentrations build up across the entire valley, and (3) occasional wintertime “gap wind” events in the eastern valley.  相似文献   

13.
14.
Long-standing measurement techniques for determining ground-level ozone (O3) and nitrogen dioxide (NO2) are known to be biased by interfering compounds that result in overestimates of high O3 and NO2 ambient concentrations under conducive conditions. An increasing near-ground O3 gradient (NGOG) with increasing height above ground level is also known to exist. Both the interference bias and NGOG were investigated by comparing data from a conventional Federal Equivalent Method (FEM) O3 photometer and an identical monitor upgraded with an “interference-free” nitric oxide O3 scrubber that alternatively sampled at 2 m and 6.2 m inlet heights above ground level (AGL). Intercomparison was also made between a conventional nitrogen oxide (NOx) chemiluminescence Federal Reference Method (FRM) monitor and a new “direct-measure” NO2 NOx 405 nm photometer at a near-road air quality measurement site. Results indicate that the O3 monitor with the upgraded scrubber recorded lower regulatory-oriented concentrations than the deployed conventional metal oxide–scrubbed monitor and that O3 concentrations 6.2 m AGL were higher than concentrations 2.0 m AGL, the nominal nose height of outdoor populations. Also, a new direct-measure NO2 photometer recorded generally lower NO2 regulatory-oriented concentrations than the conventional FRM chemiluminescence monitor, reporting lower daily maximum hourly average concentrations than the conventional monitor about 3 of every 5 days.

Implications: Employing bias-prone instruments for measurement of ambient ozone or nitrogen dioxide from inlets at inappropriate heights above ground level may result in collection of positively biased data. This paper discusses tests of new regulatory instruments, recent developments in bias-free ozone and nitrogen dioxide measurement technology, and the presence/extent of a near-ground O3 gradient (NGOG). Collection of unbiased monitor inlet height–appropriate data is crucial for determining accurate design values and meeting National Ambient Air Quality Standards.  相似文献   


15.

The objective of this study was to assess the contamination level of potentially harmful elements (PHEs) in industrial soils and how this relates to environmental magnetism. Moreover, emphasis was given to the determination of the potential mobile fractions of typically “technogenic” metals. Therefore, magnetic and geochemical parameters were determined in topsoils (0–20 cm) collected around a chemical industry in Sindos Industrial Area, Thessaloniki, Greece. Soil samples were presented significantly enriched in “technogenic” metals such Cd, Pb, and Zn, while cases of severe soil contamination were observed in sampling sites north-west of the industrial unit. Contents of Cd, Cr, Cu, Ni, Pb, Mo, Sb, Sn, and Zn in soils and pollution load index (PLI) were highly correlated with mass specific magnetic susceptibility (χ lf). Similarly, enrichment factor (EF) and geoaccumulation index (I geo) for “technogenic” Pb and Zn exhibited high positive correlation factors with χ lf. Principal component analysis (PCA) classified PHEs along with the magnetic variable (χ lf) into a common group indicating anthropogenic influence. The water extractable concentrations were substantially low, while the descending order of UBM (Unified BARGE Method) extractable concentrations in the gastric phase was Zn > Pb > As > Cd, yet Cd showed the highest bioaccessibility (almost 95%).

  相似文献   

16.
The environment and its interactions with human systems, whether economic, social, or political, are complex. Relevant drivers may disrupt system dynamics in unforeseen ways, making it difficult to predict future conditions. This kind of “deep uncertainty” presents a challenge to organizations faced with making decisions about the future, including those involved in air quality management. Scenario Planning is a structured process that involves the development of narratives describing alternative future states of the world, designed to differ with respect to the most critical and uncertain drivers. The resulting scenarios are then used to understand the consequences of those futures and to prepare for them with robust management strategies. We demonstrate a novel air quality management application of Scenario Planning. Through a series of workshops, important air quality drivers were identified. The most critical and uncertain drivers were found to be “technological development” and “change in societal paradigms.” These drivers were used as a basis to develop four distinct scenario storylines. The energy and emissions implications of each storyline were then modeled using the MARKAL energy system model. NOx emissions were found to decrease for all scenarios, largely a response to existing air quality regulations, whereas SO2 emissions ranged from 12% greater to 7% lower than 2015 emissions levels. Future-year emissions differed considerably from one scenario to another, however, with key differentiating factors being transition to cleaner fuels and energy demand reductions.

Implications: Application of scenarios in air quality management provides a structured means of sifting through and understanding the dynamics of the many complex driving forces affecting future air quality. Further, scenarios provide a means to identify opportunities and challenges for future air quality management, as well as a platform for testing the efficacy and robustness of particular management options across wide-ranging conditions.  相似文献   

17.
We investigated variations in the relative sensitivity of surface ozone formation in summer to precursor species concentrations of volatile organic compounds (VOCs) and nitrogen oxides (NOx) as inferred from the ratio of the tropospheric columns of formaldehyde to nitrogen dioxide (the “Ratio”) from the Aura Ozone Monitoring Instrument (OMI). Our modeling study suggests that ozone formation decreases with reductions in VOCs at Ratios <1 and NOx at Ratios >2; both NOx and VOC reductions may decrease ozone formation for Ratios between 1 and 2. Using this criteria, the OMI data indicate that ozone formation became: 1. more sensitive to NOx over most of the United States from 2005 to 2007 because of the substantial decrease in NOx emissions, primarily from stationary sources, and the concomitant decrease in the tropospheric column of NO2, and 2. more sensitive to NOx with increasing temperature, in part because emissions of highly reactive, biogenic isoprene increase with temperature, thus increasing the total VOC reactivity. In cities with relatively low isoprene emissions (e.g., Chicago), the data clearly indicate that ozone formation became more sensitive to NOx from 2005 to 2007. In cities with relatively high isoprene emissions (e.g., Atlanta), we found that the increase in the Ratio due to decreasing NOx emissions was not obvious as this signal was convolved with variations in the Ratio associated with the temperature dependence of isoprene emissions and, consequently, the formaldehyde concentration.  相似文献   

18.
A full-scale sequencing batch reactor (SBR) system was evaluated for its ability to remove carbon and nitrogen from swine wastewater. The SBR was operated on four, six-hour cycles each day, with each cycle consisting of 4.5 hours of “React,” 0.75 hours of “Settling”, 0.75 hours for “Draw” and “Fill.” Within each cycle, an amount of wastewater equivalent to about 5% of the reactor volume (5,500 litres) was removed and added. The SBR system was able to remove 82% of biochemical oxygen demand (BOD) and more than 75% of nitrogen. Even though the SBR effluent, with an average effluent BOD5 of about 588 mg L? 1, did not meet the discharge criteria, it enabled a reduction of the land base required for land application of swine wastewater by about 75%. Results indicated that the SBR system was a viable method for the treatment of swine wastewater.  相似文献   

19.
Urban Airshed Model-Version IV (UAM-IV) simulations on 7–8 July, 1988 for the Atlanta, Georgia, nonattainment area are used to investigate how recent changes in the National Ambient Air Quality Standard (NAAQS) and changes in boundary concentrations may affect attempts to comply with the standard through local emissions reductions. According to model results, the recently promulgated 8 h NAAQS at a level of 0.08 ppmv will require larger emission reductions to comply with the standard than those that are necessary to comply with the previous 1 h/0.12 ppmv NAAQS. Regardless of the form of the NAAQS or the magnitude of the concentrations of O3 and its precursors at the model domain boundary, UAM-IV simulations for Atlanta predict that NOx (NO+NO2) emission reductions are more effective than volatile organic compound reductions in mitigating O3 pollution. Moreover, the simulations indicate that NOx emission reductions greater than 60–75% would be required to demonstrate attainment under either form of the standard, even if boundary concentrations of O3 and its precursors were substantially reduced. Further research is necessary to determine if this weak response to emission controls is truly representative of the real atmosphere, or is a result of the meteorological conditions specific to this episode, or is an artifact of the UAM-IV model or its inputs.  相似文献   

20.
Results from a detailed analysis of sulfur dioxide (SO2) reductions achievable through “deep” physical coal cleaning (PCC) at 20 coal-fired power plants in the Ohio-Indiana-Illinois region are presented here. These plants all have capacities larger than 500 MWe, are currently without any flue gas desulfurization (FGD) systems, and burn coal of greater than l%sulfur content (in 1980). Their aggregate emissions of 2.4 million tons of SO2 per year represents 55% of the SO2 inventory for these states. The principal coal supplies for each power plant were identified and characterized as to coal seam and county of origin, so that published coal-washability data could be matched to each supplier. The SO2 reductions that would result from deep cleaning each coal (Level 4) were calculated using an Argonne computer model that assumes a weight recovery of 80%. Percentage reductions in sulfur content ranged from zero to 52%, with a mean value of 29%, and costs ranged from a low of $364/ton SO2 removed to over $2000/ton SO2 removed. Because coal suppliers to these power plants employ some voluntary coal cleaning, the anticipated emissions reduction from current levels should be near 20%. Costs then were estimated for FGD systems designed to remove the same amount of SO2 as was achieved by PCC through the use of partial scrubbing with bypass of the remaining flue gas. On this basis, PCC was more cost-effective than FGD for about 50% of the plants studied and had comparable costs for another 25% of the plants. Possible governmental actions to either encourage or mandate coal cleaning were identified and evaluated  相似文献   

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