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1.
To study the impact of emissions at an airport on local air quality, a measurement campaign at the Zurich airport was performed from 30 June 2004 to 15 July 2004. Measurements of NO, NO2, CO and CO2 were conducted with open path devices to determine real in-use emission indices of aircraft during idling. Additionally, air samples were taken to analyse the mixing ratios of volatile organic compounds (VOC). Temporal variations of VOC mixing ratios on the airport were investigated, while other air samples were taken in the plume of an aircraft during engine ignition. CO concentrations in the vicinity of the terminals were found to be highly dependent on aircraft movement, whereas NO concentrations were dominated by emissions from ground support vehicles. The measured emission indices for aircraft showed a strong dependence upon engine type. Our work also revealed differences from emission indices published in the emission data base of the International Civil Aviation Organisation. Among the VOC, reactive C2–C3 alkenes were found in significant amounts in the exhaust of an engine compared to ambient levels. Also, isoprene, a VOC commonly associated with biogenic emissions, was found in the exhaust, however it was not detected in refuelling emissions. The benzene to toluene ratio was used to discriminate exhaust from refuelling emission. In refuelling emissions, a ratio well below 1 was found, while for exhaust this ratio was usually about 1.7.  相似文献   

2.
This study develops fine temporal (seasonal, day-of-week, diurnal) and vertical allocations of anthropogenic emissions for the TRACE-P inventory and evaluates their impacts on the East Asian air quality prediction using WRF-Chem simulations in July 2001 at 30-km grid spacing against available surface measurements from EANET and NEMCC. For NO2 and SO2, the diurnal and vertical redistributions of emissions play essential roles, while the day-of-week variation is less important. When all incorporated, WRF-Chem best simulates observations of surface NO2 and SO2 concentrations, while using the default emissions produces the worst result. The sensitivity is especially large over major cities and industrial areas, where surface NO2 and SO2 concentrations are reduced by respectively 3–7 and 6–12 ppbv when using the scaled emissions. The incorporation of all the three redistributions of emissions simulates surface O3 concentrations higher by 4–8 ppbv at night and 2–4 ppbv in daytime over broad areas of northern, eastern and central China. To this sensitivity, the diurnal redistribution contributes more than the other two.  相似文献   

3.
This work compares the WRF/Chem (Weather Research and Forecasting – Chemistry) simulated O3 concentrations in the Mexico City Metropolitan Area (MCMA) with measurements from the ground-based RAMA network during the MILAGRO (Megacity Initiative: Local and Global Research Observations) period. The model resolves the observations reasonably well in terms of diurnal cycle and mean magnitude as reflected by high correlation coefficients and low root-mean-square errors. Stations located in the center of the MCMA generally exhibit higher correlation coefficients and lower model biases than those stations located in the peripheral of the MCMA. Large temporal variations in the observed and simulated O3 concentrations are noted from station to station during the MILAGRO period. Sensitivity analyses of O3 concentrations to changes in NOx and VOC emissions rates suggest that O3 production in the MCMA is VOC-sensitive, and VOC-emissions reduction appears to be an effective strategy for reducing high surface O3 concentrations in the MCMA.  相似文献   

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Sensitivity of ozone (O3) concentrations in the Mexico City area to diurnal variations of surface air pollutant emissions is investigated using the WRF/Chem model. Our analysis shows that diurnal variations of nitrogen oxides (NOx = NO + NO2) and volatile organic compound (VOC) emissions play an important role in controlling the O3 concentrations in the Mexico City area. The contributions of NOx and VOC emissions to daytime O3 concentrations are very sensitive to the morning emissions of NOx and VOCs. Increase in morning NOx emissions leads to decrease in daytime O3 concentrations as well as the afternoon O3 maximum, while increase in morning VOC emissions tends to increase in O3 concentrations in late morning and early afternoon, indicating that O3 production in Mexico City is under VOC-limited regime. It is also found that the nighttime O3 is independent of VOCs, but is sensitive to NOx. The emissions of VOCs during other periods (early morning, evening, and night) have only small impacts on O3 concentrations, while the emissions of NOx have important impacts on O3 concentrations in the evening and the early morning.This study suggests that shifting emission pattern, while keeping the total emissions unchanged, has important impacts on air quality. For example, delaying the morning emission peak from 8 am to 10 am significantly reduced the morning peaks of NOx and VOCs, as well as the afternoon O3 maxima. It suggests that without reduction of total emission, the daytime O3 concentrations can be significantly reduced by changing the diurnal variations of the emissions of O3 precursors.  相似文献   

6.
This paper evaluates the ranking of 21 priority air pollutants with three indicator schemes: environmental pressure indicator (EPI), environmental quality indicator (EQI), and human health effect indicator (HEI). The EPI and EQI compare the emissions and concentrations with the target emissions and target concentrations, respectively. The HEI comprehends the steps from cause (i.e. national emissions) to effect (i.e. human health effects), and is the total human health burden, expressed in Disability Adjusted Life Years per year of exposure (DALYs year?1). We estimated a health burden in the Netherlands of 41 × 103 DALYs year?1 caused by Dutch air emissions of PM10 and its precursors in the year 2003. The burden due to 17 carcinogenic substances emitted to air, was much lower (140 DALYs year?1). In contrast, when the same substances were evaluated regarding environmental pressure and environmental quality, carbon tetrachloride (pressure) and benzo[a]pyrene (quality) were of highest importance, whereas the importance of PM10 was substantially lower. This result is remarkable, because for the majority of substances evaluated, the target concentrations and target emissions are based on preventing human health damage. The differences in relevance are explained by the different weighting of interests in the indicators. The HEI is based on concentration–response relations, whereas the EPI and EQI also depend on other, policy-based, principles and on technical feasibility. Therefore, to effectively prioritize emission reduction measures in policy-making, substances should not only be evaluated as to whether emission targets and environmental quality targets are reached, but they should be evaluated regarding their human health impact as well. In this context, the HEI is a suitable indicator to evaluate the human health impact.  相似文献   

7.
There is a dearth of information on dust emissions from sources that are unique to the U.S. Department of Defense testing and training activities. However, accurate emissions factors are needed for these sources so that military installations can prepare accurate particulate matter (PM) emission inventories. One such source, coarse and fine PM (PM10 and PM2.5) emissions from artillery backblast testing on improved gun positions, was characterized at the Yuma Proving Ground near Yuma, AZ, in October 2005. Fugitive emissions are created by the shockwave from artillery pieces, which ejects dust from the surface on which the artillery is resting. Other contributions of PM can be attributed to the combustion of the propellants. For a 155-mm howitzer firing a range of propellant charges or zones, amounts of emitted PM10 ranged from -19 g of PM10 per firing event for a zone 1 charge to 92 g of PM10 per firing event for a zone 5. The corresponding rates for PM2.5 were approximately 9 g of PM2.5 and 49 g of PM2.5 per firing. The average measured emission rates for PM1o and PM2.5 appear to scale with the zone charge value. The measurements show that the estimated annual contributions of PM10 (52.2 t) and PM2.5 (28.5 t) from artillery backblast are insignificant in the context of the 2002 U.S. Environment Protection Agency (EPA) PM emission inventory. Using national-level activity data for artillery fire, the most conservative estimate is that backblast would contribute the equivalent of 5 x 10(-4) % and 1.6 x 10(-3)% of the annual total PM10 and PM2.5 fugitive dust contributions, respectively, based on 2002 EPA inventory data.  相似文献   

8.
Polychlorinated biphenyls (PCBs) were banned in the United States in 1979, and since then a significant decline in their release to the environment has been observed. This decline has now reached a plateau. Several new regulatory programs have been put in place to further reduce PCB emissions/releases. However, our ability to measure the effectiveness of these regulatory/voluntary programs and to support regional fate/transport and source/receptor modeling efforts depend on reliable emission information. In this study, we attempt to improve the emission inventory for PCBs by compiling and analyzing the multimedia total PCB emission/release data reported for the U.S Great Lakes states for each year from 1990 to 2000. Although Toxic Release Inventory (TRI), National Emissions Inventory (NEI), Great Lakes Regional Air Toxic Emissions Inventory (GLRATEI), and Integrated Atmospheric Deposition Network (IADN) data formed the basis of estimating air emissions, we used the TRI, National Response Center (NRC), and PCB transformer inventory data to estimate PCB releases to land. We used the Permit Compliance System and NRC data to obtain estimates of PCB discharges to water systems in the Great Lakes states. The Remedial Action Plans for each area of concern were the primary source for estimating PCB loads of dredged sediments. On the basis of the NEI, IADN, and GLRATEI data, the total air emissions within the decade were approximately 126 t. The regionwide discharges to water systems and releases to land in the form of landfills and accidental spills in 1990-2000 were estimated as approximately 170 and 3225 t, respectively. We estimated that approximately 1.3 million t of PCB-contaminated sediment were removed or targeted for removal in five lakes of the U.S. portion of the Great Lakes basin. We stress that these estimates were based on reported amounts and the unreported PCB releases/emissions could result in significantly higher estimates.  相似文献   

9.
The Models-3 Community Multiscale Air Quality (CMAQ) Modeling System and the Particulate Matter Comprehensive Air Quality Model with extensions (PMCAMx) were applied to simulate the period June 29-July 10, 1999, of the Southern Oxidants Study episode with two nested horizontal grid sizes: a coarse resolution of 32 km and a fine resolution of 8 km. The predicted spatial variations of ozone (O3), particulate matter with an aerodynamic diameter less than or equal to 2.5 microm (PM2.5), and particulate matter with an aerodynamic diameter less than or equal to 10 microm (PM10) by both models are similar in rural areas but differ from one another significantly over some urban/suburban areas in the eastern and southern United States, where PMCAMx tends to predict higher values of O3 and PM than CMAQ. Both models tend to predict O3 values that are higher than those observed. For observed O3 values above 60 ppb, O3 performance meets the U.S. Environmental Protection Agency's criteria for CMAQ with both grids and for PMCAMx with the fine grid only. It becomes unsatisfactory for PMCAMx and marginally satisfactory for CMAQ for observed O3 values above 40 ppb. Both models predict similar amounts of sulfate (SO4(2-)) and organic matter, and both predict SO4(2-) to be the largest contributor to PM2.5. PMCAMx generally predicts higher amounts of ammonium (NH4+), nitrate (NO3-), and black carbon (BC) than does CMAQ. PM performance for CMAQ is generally consistent with that of other PM models, whereas PMCAMx predicts higher concentrations of NO3-, NH4+, and BC than observed, which degrades its performance. For PM10 and PM2.5 predictions over the southeastern U.S. domain, the ranges of mean normalized gross errors (MNGEs) and mean normalized bias are 37-43% and -33-4% for CMAQ and 50-59% and 7-30% for PMCAMx. Both models predict the largest MNGEs for NO3- (98-104% for CMAQ 138-338% for PMCAMx). The inaccurate NO3- predictions by both models may be caused by the inaccuracies in the ammonia emission inventory and the uncertainties in the gas/particle partitioning under some conditions. In addition to these uncertainties, the significant PM overpredictions by PMCAMx may be attributed to the lack of wet removal for PM and a likely underprediction in the vertical mixing during the daytime.  相似文献   

10.
Principles are presented for standardization and establishment of maximum permissible emissions (MPE) into the atmosphere in accordance with theoretical and experimental investigations of pollutant diffusion from sources of various types, accounting for meteorological and topographical conditions. MPE refers to the amount of pollutants from a single source that together with other neighbouring sources give rise to air pollution concentrations that do not exceed the air quality standard. Due to a lack of confidence in theories it is impossible at present to prove the establishment of MPE and our present technical knowledge supports only a gradual decrease of emissions and determination of temporarily agreed emissions (TAE). For determination of MPE and TAE from multiple urban sources, calculation and analysis of their total concentration field are performed. The physical bases of the methods for standardization of industrial emissions officially adopted in the U.S.S.R. for practical use are presented. It is considered how standardization and establishment of MPE and control on their fulfillment are organized in the U.S.S.R.  相似文献   

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Impact of the excited nitrogen dioxide (NO21) chemistry on air quality in the U.S. is examined using the Community Multiscale Air Quality (CMAQ) model for a summer month. Model simulations were conducted with and without the NO21 chemistry. The largest impact of the NO21 chemistry in the eastern U.S. occurred in the northeast and in the western U.S. occurred in Los Angeles. While the single largest daily maximum 8-h ozone (O3) increased by 9 ppbv in eastern U.S. and 6 ppbv in western U.S., increases on most days were much lower. No appreciable change in model performance statistics for surface-level O3 predictions relative to measurements is noted between simulations with and without the NO21 chemistry. Based on model calculations using current estimates of tropospheric emission burden, the NO21 chemistry can increase the monthly mean daytime hydroxyl radicals (OH) and nitrous acid (HONO) by a maximum of 28% and 100 pptv, respectively.  相似文献   

14.
The sensitivity of the CHIMERE model to emission reduction scenarios on particulate matter PM2.5 and ozone (O3) in Northern Italy is studied. The emissions of NOx, PM2.5 SO2, VOC or NH3 were reduced by 50% for different source sectors for the Lombardy region, together with 5 additional scenarios to estimate the effect of local measures on improving the air quality for the Po valley area. Firstly, we evaluate the model performance by comparing calculated surface aerosol concentrations for the standard case (no emission reductions) with observations for January and June 2005. Calculated monthly mean PM10 concentrations are in general underestimated. For June, modelled PM10 concentrations slightly overestimate the measurements. Calculated monthly mean SO4, NO3?, NH4+ concentrations are in good agreement with the observations for January and June. Secondly, the model sensitivity of emission reduction scenarios on PM2.5 and O3 calculated concentrations for the Po valley area is evaluated. The most effective scenarios to abate PM2.5 concentration are based on the SNAP2 (non-industrial combustion plants) and SNAP7 (road traffic) sectors, for which the NOx and PM2.5 emissions are reduced by 50%. The number of days that the 2015 PM2.5 limit value of 25 μg m?3 in Milan is exceeded by reducing primary PM2.5 and NOx emissions for SNAP2 and 7 by 50%, does not change in January when compared to the standard case for the Milan area. It appears that 40% of the PM2.5 concentration in the greater Milan area is caused by the emissions surrounding the Lombardy region and from the model boundary conditions.This study also showed that a more effective pollutant reduction (emissions) per ton of pollutant reduced (concentrations) for the greater Milan area is obtained by reducing the primary PM2.5 emissions for SNAP7 by 50%. The most effective scenario on PM2.5 decrease for which precursor emissions are reduced is achieved by reducing SO2 emissions by 50% for SNAP7.Our study showed that during summer time, the largest reductions in O3 concentrations are achieved for SNAP7 emission reductions, when volatile organic compounds (VOCs) are reduced by 50%.  相似文献   

15.
Mobile sources significantly contribute to ambient concentrations of airborne particulate matter (PM). Source apportionment studies for PM10 (PM < or = 10 microm in aerodynamic diameter) and PM2.5 (PM < or = 2.5 microm in aerodynamic diameter) indicate that mobile sources can be responsible for over half of the ambient PM measured in an urban area. Recent source apportionment studies attempted to differentiate between contributions from gasoline and diesel motor vehicle combustion. Several source apportionment studies conducted in the United States suggested that gasoline combustion from mobile sources contributed more to ambient PM than diesel combustion. However, existing emission inventories for the United States indicated that diesels contribute more than gasoline vehicles to ambient PM concentrations. A comprehensive testing program was initiated in the Kansas City metropolitan area to measure PM emissions in the light-duty, gasoline-powered, on-road mobile source fleet to provide data for PM inventory and emissions modeling. The vehicle recruitment design produced a sample that could represent the regional fleet, and by extension, the national fleet. All vehicles were recruited from a stratified sample on the basis of vehicle class (car, truck) and model-year group. The pool of available vehicles was drawn primarily from a sample of vehicle owners designed to represent the selected demographic and geographic characteristics of the Kansas City population. Emissions testing utilized a portable, light-duty chassis dynamometer with vehicles tested using the LA-92 driving cycle, on-board emissions measurement systems, and remote sensing devices. Particulate mass emissions were the focus of the study, with continuous and integrated samples collected. In addition, sample analyses included criteria gases (carbon monoxide, carbon dioxide, nitric oxide/nitrogen dioxide, hydrocarbons), air toxics (speciated volatile organic compounds), and PM constituents (elemental/organic carbon, metals, semi-volatile organic compounds). Results indicated that PM emissions from the in-use fleet varied by up to 3 orders of magnitude, with emissions generally increasing for older model-year vehicles. The study also identified a strong influence of ambient temperature on vehicle PM mass emissions, with rates increasing with decreasing temperatures.  相似文献   

16.
Fine particulate matter (PM2.5) air pollution has been linked to adverse health impacts, and combustion sources including residential wood-burning may play an important role in some regions. Recent evidence suggests that indoor air quality may improve in homes where older, non-certified wood stoves are exchanged for lower emissions EPA-certified alternatives. As part of a wood stove exchange program in northern British Columbia, Canada, we sampled outdoor and indoor air at 15 homes during 6-day sampling sessions both before and after non-certified wood stoves were exchanged. During each sampling session two consecutive 3-day PM2.5 samples were collected onto Teflon filters, which were weighed and analyzed for the wood smoke tracer levoglucosan. Residential PM2.5 infiltration efficiencies (Finf) were estimated from continuous light scattering measurements made with nephelometers, and estimates of Finf were used to calculate the outdoor- and indoor-generated contributions to indoor air. There was not a consistent relationship between stove technology and outdoor or indoor concentrations of PM2.5 or levoglucosan. Mean Finf estimates were low and similar during pre- and post-exchange periods (0.32 ± 0.17 and 0.33 ± 0.17, respectively). Indoor sources contributed the majority (~65%) of the indoor PM2.5 concentrations, independent of stove technology, although low indoor-outdoor levoglucosan ratios (median ≤ 0.19) and low indoor PM2.5-levoglucosan correlations (r ≤ 0.19) suggested that wood smoke was not a major indoor PM2.5 source in most of these homes. In summary, despite the potential for extensive wood stove exchange programs to reduce outdoor PM2.5 concentrations in wood smoke-impacted communities, we did not find a consistent relationship between stove technology upgrades and indoor air quality improvements in homes where stoves were exchanged.  相似文献   

17.
During autumn, 2006, variation in the frequency of aerosol nucleation events, as inferred from nanoparticle growth events, and associated hygroscopicity were investigated as a function of air mass transport history at a mixed deciduous forest in central Virginia, U.S. Above-canopy size distributions of aerosols between 0.012 and 0.700 μm diameter, size-resolved particle hygroscopicity at eight dry diameters between 0.012 and 0.400 μm, and cloud condensation nuclei (CCN) activity were characterized. Air mass back trajectories were clustered to identify source regions. Growth events were most frequent in fast-moving air masses (mean = 9 m s?1) that originated over the north central U.S. Under these flow regimes, mean values for preexisting sub-μm aerosol number concentrations (4700 cm?3), corresponding surface area (142 μm2 cm?3), air temperature (6.2 °C), and relative humidity (RH, 49.4%) were relatively low compared to other regimes. Under stagnant flow conditions (mean = 3 m s?1), mean number concentrations were higher (>6000 cm?3) and size fractions <0.1 μm diameter exhibited enhanced hygroscopicity compared to other source regions. These results indicate that precursors emitted into relatively clean, cold, and dry air transported over the southeastern U.S. reacted to form condensable intermediates that subsequently produced new aerosols via nucleation and growth. This pathway was an important source for CCN. During events in October, nanoparticles were produced in greater numbers and grew more rapidly compared to November and December.  相似文献   

18.
The emission, transport, deposition and eventual fate of mercury (Hg) in the Mediterranean area has been studied using a modified version of the Weather Research and Forecasting model coupled with Chemistry (WRF/Chem). This model version has been developed specifically with the aim to simulate the atmospheric processes determining atmospheric Hg emissions, concentrations and deposition online at high spatial resolution. For this purpose, the gas phase chemistry of Hg and a parametrised representation of atmospheric Hg aqueous chemistry have been added to the regional acid deposition model version 2 chemical mechanism in WRF/Chem. Anthropogenic mercury emissions from the Arctic Monitoring and Assessment Programme included in the emissions preprocessor, mercury evasion from the sea surface and Hg released from biomass burning have also been included. Dry and wet deposition processes for Hg have been implemented. The model has been tested for the whole of 2009 using measurements of total gaseous mercury from the European Monitoring and Evaluation Programme monitoring network. Speciated measurement data of atmospheric elemental Hg, gaseous oxidised Hg and Hg associated with particulate matter, from a Mediterranean oceanographic campaign (June 2009), has permitted the model’s ability to simulate the atmospheric redox chemistry of Hg to be assessed. The model results highlight the importance of both the boundary conditions employed and the accuracy of the mercury speciation in the emission database. The model has permitted the reevaluation of the deposition to, and the emission from, the Mediterranean Sea. In light of the well-known high concentrations of methylmercury in a number of Mediterranean fish species, this information is important in establishing the mass balance of Hg for the Mediterranean Sea. The model results support the idea that the Mediterranean Sea is a net source of Hg to the atmosphere and suggest that the net flux is ≈30 Mg year?1 of elemental Hg.  相似文献   

19.
Vegetation composition and biomass were surveyed for three specific sites in Atlanta, GA; near Rhinelander, WI; and near Hayden, CO. At each research site emissions of biogenic volatile organic compounds (BVOCs) from the dominant vegetation species were sampled by enclosing branches in bag enclosure systems and sampling the equilibrium head space onto multi-stage solid adsorbent cartridges. Analysis was performed using a thermal desorption technique with gas chromatography (GC) separation and mass spectrometry (MS) detection. Identification of BVOCs covering the GC retention index range (stationary phase DB-1) from approximately 400 to 1400 was achieved (volatilities C4-C14).  相似文献   

20.
It is estimated that there is sufficient in-state “technically” recoverable biomass to support nearly 4000 MW of bioelectricity generation capacity. This study assesses the emissions of greenhouse gases and air pollutants and resulting air quality impacts of new and existing bioenergy capacity throughout the state of California, focusing on feedstocks and advanced technologies utilizing biomass resources predominant in each region. The options for bioresources include the production of bioelectricity and renewable natural gas (NG). Emissions of criteria pollutants and greenhouse gases are quantified for a set of scenarios that span the emission factors for power generation and the use of renewable natural gas for vehicle fueling. Emissions are input to the Community Multiscale Air Quality (CMAQ) model to predict regional and statewide temporal air quality impacts from the biopower scenarios. With current technology and at the emission levels of current installations, maximum bioelectricity production could increase nitrogen oxide (NOx) emissions by 10% in 2020, which would cause increases in ozone and particulate matter concentrations in large areas of California. Technology upgrades would achieve the lowest criteria pollutant emissions. Conversion of biomass to compressed NG (CNG) for vehicles would achieve comparable emission reductions of criteria pollutants and minimize emissions of greenhouse gases (GHG). Air quality modeling of biomass scenarios suggest that applying technological changes and emission controls would minimize the air quality impacts of bioelectricity generation. And a shift from bioelectricity production to CNG production for vehicles would reduce air quality impacts further. From a co-benefits standpoint, CNG production for vehicles appears to provide the best benefits in terms of GHG emissions and air quality.

Implications:?This investigation provides a consistent analysis of air quality impacts and greenhouse gas emissions for scenarios examining increased biomass use. Further work involving economic assessment, seasonal or annual emissions and air quality modeling, and potential exposure analysis would help inform policy makers and industry with respect to further development and direction of biomass policy and bioenergy technology alternatives needed to meet energy and environmental goals in California.  相似文献   

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