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1.
A modeling system consisting of MM5, Calmet, and Calgrid was used to investigate the sensitivity of anthropogenic volatile organic compound (VOC) and oxides of nitrogen (NOx) reductions on ozone formation within the Cascadia airshed of the Pacific Northwest. An ozone episode that occurred on July 11-14, 1996, was evaluated. During this event, high ozone levels were recorded at monitors downwind of Seattle, WA, and Portland, OR, with one monitor exceeding the 1 hr/120 ppb National Ambient Air Quality Standard (at 148 ppb), and six monitors above the proposed 8 hr/80 ppb standard (at 82-130 ppb). For this particular case, significant emissions reductions, between 25 and 75%, would be required to decrease peak ozone concentrations to desired levels. Reductions in VOC emissions alone, or a combination of reduced VOC and NOx emissions, were generally found to be most effective; reducing NOx emissions alone resulted in increased ozone in the Seattle area. When only VOC emissions were curtailed, ozone reductions occurred in the immediate vicinity of densely populated areas, while NOx reductions resulted in more widespread ozone reductions.  相似文献   

2.
Natural emissions adopted in current regional air quality modeling are updated to better describe natural background ozone and PM concentrations for North America. The revised natural emissions include organosulfur from the ocean, NO from lightning, sea salt, biogenic secondary organic aerosol (SOA) precursors, and pre-industrial levels of background methane. The model algorithm for SOA formation was also revised. Natural background ozone concentrations increase by up to 4 ppb in annual average over the southeastern US and Gulf of Mexico due to added NO from lightning while the revised biogenic emissions produced less ozone in the central and western US. Natural PM2.5 concentrations generally increased with the revised natural emissions. Future year (2018) simulations were conducted for several anthropogenic emission reduction scenarios to assess the impact of the revised natural emissions on anthropogenic emission control strategies. Overall, the revised natural emissions did not significantly alter the ozone responses to the emissions reductions in 2018. With revised natural emissions, ozone concentrations were slightly less sensitive to reducing NOx in the southeastern US than with the current natural emissions due to higher NO from lightning. The revised natural emissions have little impact on modeled PM2.5 responses to anthropogenic emission reductions. However, there are substantial uncertainties in current representations of natural sources in air quality models and we recommend that further study is needed to refine these representations.  相似文献   

3.
A spatially and temporally resolved biogenic hydrocarbon and nitrogen oxides (NOx) emissions inventory has been developed for a region along the Mexico-U.S. border area. Average daily biogenic non-methane organic gases (NMOG) emissions for the 1700 x 1000 km2 domain were estimated at 23,800 metric tons/day (62% from Mexico and 38% from the United States), and biogenic NOx was estimated at 1230 metric tons/day (54% from Mexico and 46% from the United States) for the July 18-20, 1993, ozone episode. The biogenic NMOG represented 74% of the total NMOG emissions, and biogenic NOx was 14% of the total NOx. The CIT photochemical airshed model was used to assess how biogenic emissions impact air quality. Predicted ground-level ozone increased by 5-10 ppb in most rural areas, 10-20 ppb near urban centers, and 20-30 ppb immediately downwind of the urban centers compared to simulations in which only anthropogenic emissions were used. A sensitivity analysis of predicted ozone concentration to emissions was performed using the decoupled direct method for three dimensional air quality models (DDM-3D). The highest positive sensitivity of ground-level ozone concentration to biogenic volatile organic compound (VOC) emissions (i.e., increasing biogenic VOC emissions results in increasing ozone concentrations) was predicted to be in locations with high NOx levels, (i.e., the urban areas). One urban center--Houston--was predicted to have a slight negative sensitivity to biogenic NO emissions (i.e., increasing biogenic NO emissions results in decreasing local ozone concentrations). The highest sensitivities of ozone concentrations to on-road mobile source VOC emissions, all positive, were mainly in the urban areas. The highest sensitivities of ozone concentrations to on-road mobile source NOx emissions were predicted in both urban (either positive or negative sensitivities) and rural (positive sensitivities) locations.  相似文献   

4.
It is widely accepted that the ozone concentrations experienced during photochemical episodes over large areas of Europe may exceed levels at which adverse environmental effects could be expected. These peak ozone concentrations can be reduced by controlling atmospheric emissions of the hydrocarbon and nitrogen oxide precursors. For ozone control to be successful over the spatial scale of Europe, long term international cooperation is required in the formulation of emission abatement strategies. A significant barrier to rapid progress has been the complexity of the processes that describe ozone formation. Highly sophisticated computer models of chemistry and transport have, up to now, been the only means to study the impact of abatement strategies. An alternative approach has been adopted here involving the development of a simplified long range transport model for ozone based on the analysis of over 60 experimental runs of a photochemical trajectory model applied to a wide range of hydrocarbon-nitrogen oxide emission combinations. Using the ozone-precursor relationship obtained, it has been possible to examine various policy options in the European context. Although taken together, three illustrative emission control scenarios reduce NO(x) and hydrocarbon emissions substantially through controls on motor vehicle exhaust, large combustion plant and solvent usage, a significant potential for photochemical ozone formation and long range transport may still remain after their implementation. The extents of precursor emission abatement that will be required, if the potential for ozone formation is to be reduced below published air quality criteria guidelines or critical levels, have been determined for each European country. The implied reductions in NO(x) and hydrocarbons relative to current levels amount to between 50 and 90%.  相似文献   

5.
An ozone abatement strategy for the South Coast Air Basin (SoCAB) has been proposed by the South Coast Air Quality Management District (SCAQMD) and the California Air Resources Board (ARB). The proposed emissions reduction strategy is focused on the reduction of nitrogen oxide (NOx) emissions by the year 2030. Two high PM2.5 concentration episodes with high ammonium nitrate compositions occurring during September and November 2008 were simulated with the Community Multi-scale Air Quality model (CMAQ). All simulations were made with same meteorological files provided by the SCAQMD to allow them to be more directly compared with their previous modeling studies. Although there was an overall under-prediction bias, the CMAQ simulations were within an overall normalized mean error of 50%; a range that is considered acceptable performance for PM modeling. A range of simulations of these episodes were made to evaluate sensitivity to NOx and ammonia emissions inputs for the future year 2030. It was found that the current ozone control strategy will reduce daily average PM2.5 concentrations. However, the targeted NOx reductions for ozone were not found to be optimal for reducing PM2.5 concentrations. Ammonia emission reductions reduced PM2.5 and this might be considered as part of a PM2.5 control strategy.

Implications: The SCAQMD and the ARB have proposed an ozone abatement strategy for the SoCAB that focuses on NOx emission reductions. Their strategy will affect both ozone and PM2.5. Two episodes that occurred during September and November 2008 with high PM2.5 concentrations and high ammonium nitrate composition were selected for simulation with different levels of nitrogen oxide and ammonia emissions for the future year 2030. It was found that the ozone control strategy will reduce maximum daily average PM2.5 concentrations but its effect on PM2.5 concentrations is not optimal.  相似文献   


6.
A computer model called the Ozone Risk Assessment Model (ORAM) was developed to evaluate the health effects caused by ground-level ozone (O3) exposure. ORAM was coupled with the U.S. Environmental Protection Agency's (EPA) Third-Generation Community Multiscale Air Quality model (Models-3/CMAQ), the state-of-the-art air quality model that predicts O3 concentration and allows the examination of various scenarios in which emission rates of O3 precursors (basically, oxides of nitrogen [NOx] and volatile organic compounds) are varied. The principal analyses in ORAM are exposure model performance evaluation, health-effects calculations (expected number of respiratory hospital admissions), economic valuation, and sensitivity and uncertainty analysis through a Monte Carlo simulation. As a demonstration of the system, ORAM was applied to the eastern Tennessee region, and the entire O3 season was simulated for a base case (typical emissions) and three different emission scenarios. The results indicated that a synergism occurs when reductions in NOx emissions from mobile and point sources were applied simultaneously. A 12.9% reduction in asthma hospital admissions is expected when both mobile and point source NOx emissions are reduced (50 and 70%, respectively) versus a 5.8% reduction caused by mobile source and a 3.5% reduction caused by point sources when these emission sources are reduced individually.  相似文献   

7.
This paper analyzes the benefits and costs of policies to reduce NOx emissions from electricity generation in the United States. Because emissions of NO contribute to the high concentration of atmospheric ozone in the eastern states associated with health hazards, the U.S. Environmental Protection Agency (EPA) has called on eastern states to formulate state implementation plans (SIPs) for reducing NOx emissions. Our analysis considers three NOx reduction scenarios: a summer seasonal cap in the eastern states covered by EPA's NOx SIP Call, an annual cap in the same SIP Call region, and a national annual cap. All scenarios allow for emissions trading. Although EPA's current policy is to implement a seasonal cap in the SIP Call region, this analysis indicates that an annual cap in the SIP Call region would yield about $400 million more in net benefits (benefits less costs) than would a seasonal policy, based on particulate-related health effects only. An annual cap in the SIP Call region is also the policy that is most likely to achieve benefits in excess of costs. Consideration of omissions from this accounting, including the potential benefits from reductions in ozone concentrations, strengthens the finding that an annual program offers greater net benefits than does a seasonal program.  相似文献   

8.
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   

9.
The role of emissions of volatile organic compounds and nitric oxide from biogenic sources is becoming increasingly important in regulatory air quality modeling as levels of anthropogenic emissions continue to decrease and stricter health-based air quality standards are being adopted. However, considerable uncertainties still exist in the current estimation methodologies for biogenic emissions. The impact of these uncertainties on ozone and fine particulate matter (PM2.5) levels for the eastern United States was studied, focusing on biogenic emissions estimates from two commonly used biogenic emission models, the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the Biogenic Emissions Inventory System (BEIS). Photochemical grid modeling simulations were performed for two scenarios: one reflecting present day conditions and the other reflecting a hypothetical future year with reductions in emissions of anthropogenic oxides of nitrogen (NOx). For ozone, the use of MEGAN emissions resulted in a higher ozone response to hypothetical anthropogenic NOx emission reductions compared with BEIS. Applying the current U.S. Environmental Protection Agency guidance on regulatory air quality modeling in conjunction with typical maximum ozone concentrations, the differences in estimated future year ozone design values (DVF) stemming from differences in biogenic emissions estimates were on the order of 4 parts per billion (ppb), corresponding to approximately 5% of the daily maximum 8-hr ozone National Ambient Air Quality Standard (NAAQS) of 75 ppb. For PM2.5, the differences were 0.1-0.25 microg/m3 in the summer total organic mass component of DVFs, corresponding to approximately 1-2% of the value of the annual PM2.5 NAAQS of 15 microg/m3. Spatial variations in the ozone and PM2.5 differences also reveal that the impacts of different biogenic emission estimates on ozone and PM2.5 levels are dependent on ambient levels of anthropogenic emissions.  相似文献   

10.
The importance of the interaction between chemistry and dynamics in the upper troposphere and lower stratosphere for chemical species like ozone is investigated using two chemistry-climate models and a Lagrangian trajectory model. Air parcels from the upper troposphere, i.e. regions of lightning and aircraft emissions, are able to be transported into the lowermost stratosphere (LMS). Trajectory calculations suggest that the main transport pathway runs via the inter tropical convergence zone, across the tropical tropopause and then to higher latitudes, i.e. into the LMS. NOx from aircraft emissions at mid-latitudes are unlikely to perturb the LMS since they are washed-out while still in the troposphere. In contrast, NOx from tropical lightning has the chance to accumulate in the LMS. Because of the longer residence times of NOx in the LMS, compared to the upper troposphere, this excess NOx from lightning has the potential to form ozone in the LMS, which then is transported back to the troposphere at mid-latitudes. In the models, around 10% of the ozone concentration and 50% of the NOx concentration in the northern hemisphere LMS is produced by lightning NOx At least 5% of the ozone concentration and 35% the NOx concentration at 150 hPa at mid-latitudes originates from tropical lightning in the climate-chemistry simulations.  相似文献   

11.
A high ozone event in the Houston–Galveston–Brazoria area was utilized to study the shortcomings of the current air quality models. To improve the baseline simulations with the Comprehensive Air quality Model with Extensions (CAMx) for developing the state implementation plan, the Texas Commission on Environmental Quality (TCEQ) imputed emissions of highly reactive volatile organic compounds (HRVOCs) by scaling the amount of fugitive emissions of olefins to co-emitted NOx from selected point sources, effectively multiplying by 3–12 times over the regular inventory values. In this paper, CAMx and the Community Multiscale Air Quality (CMAQ) model were used to determine if the imputed HRVOC emissions were consistent with the observed atmospheric conditions. With the base emissions, CMAQ and CAMx both with the Carbon-Bond 4 (CB-4) mechanism simulated similar ozone concentrations. But with the imputed HRVOC emissions, CMAQ predicted lower ozone peaks than CAMx in the vicinity and downwind of the Ship Channel and other highly HRVOC-rich areas. Based on analyses of sensitivity simulations of CMAQ with different emission inputs and vertical diffusion algorithms in the model, we found that the modeled atmosphere lacked reactivity to produce the observed high ozone event. Although the imputed HRVOC emissions improved ozone prediction at the surface sites, but the ethylene concentrations were not consistent with the measurements at the super sites (La Porte and Clinton) and by NOAA aircraft. Several sensitivity tests designed to provide additional radicals into the system and other research results suggested that the lack of reactivity may need to be corrected by targeted, and probably of episodic, increase of HRVOC emissions, from the sources in the Houston Ship Channel. Additional investigation of the ozone production efficiency for different chemical mechanisms is necessary to pinpoint the emissions uncertainty issues.  相似文献   

12.
ABSTRACT

A modeling system consisting of MM5, Calmet, and Calgrid was used to investigate the sensitivity of anthropogenic volatile organic compound (VOC) and oxides of nitrogen (NOx) reductions on ozone formation within the Cascadia airshed of the Pacific Northwest. An ozone episode that occurred on July 11-14, 1996, was evaluated. During this event, high ozone levels were recorded at monitors downwind of Seattle, WA, and Portland, OR, with one monitor exceeding the 1 hr/120 ppb National Ambient Air Quality Standard (at 148 ppb), and six monitors above the proposed 8 hr/80 ppb standard (at 82-130 ppb). For this particular case, significant emissions reductions, between 25 and 75%, would be required to decrease peak ozone concentrations to desired levels. Reductions in VOC emissions alone, or a combination of reduced VOC and NOx emissions, were generally found to be most effective; reducing NOx emissions alone resulted in increased ozone in the Seattle area. When only VOC emissions were curtailed, ozone reductions occurred in the immediate vicinity of densely populated areas, while NOx reductions resulted in more widespread ozone reductions.  相似文献   

13.
Ambient observations have indicated that high concentrations of ozone observed in the Houston/Galveston area are associated with plumes of highly reactive hydrocarbons, mixed with NOx, from industrial facilities. Ambient observations and industrial process data, such as mass flow rates for industrial flares, indicate that the VOCs associated with these industrial emissions can have significant temporal variability. To characterize the effect of this variability in emissions on ozone formation in Houston, data were collected on the temporal variability of industrial emissions or emission surrogates (e.g., mass flow rates to flares). The observed emissions variability was then used to construct regionwide emission inventories with variable industrial emissions, and the impacts of the variability on ozone formation were examined for two types of meteorological conditions, both of which lead to high ozone concentrations in Houston. The air quality simulations indicate that variability in industrial emissions has the potential to cause increases and decreases of 10–52 ppb (13–316%), or more, in ozone concentration. The largest of these differences are restricted to regions of 10–20 km2, but the variability also has the potential to increase regionwide maxima in ozone concentrations by up to 12 ppb.  相似文献   

14.
The city of Santiago, Chile experiences frequent high pollution episodes and as a consequence very high ozone concentrations, which are associated with health problems including increasing daily mortality and hospital admissions for respiratory illnesses. The development of ozone abatement strategies requires the determination of the potential of each pollutant to produce ozone, taking into account known mechanisms and chemical kinetics in addition to ambient atmospheric conditions. In this study, the photochemical formation of ozone during a summer campaign carried out from March 8–20, 2005 has been investigated using an urban photochemical box model based on the Master Chemical Mechanism (MCMv3.1). The MCM box model has been constrained with 10 min averages of simultaneous measurements of HONO, HCHO, CO, NO, j(O1D), j(NO2), 31 volatile organic compounds (VOCs) and meteorological parameters. The O3–NOx–VOC sensitivities have been determined by simulating ozone formation at different VOC and NOx concentrations. Ozone sensitivity analyses showed that photochemical ozone formation is VOC-limited under average summertime conditions in Santiago. The results of the model simulations have been compared with a set of potential empirical indicator relationships including H2O2/HNO3, HCHO/NOy and O3/NOz. The ozone forming potential of each measured VOC has been determined using the MCM box model. The impacts of the above study on possible summertime ozone control strategies in Santiago are discussed.  相似文献   

15.
In this paper, the NOx emission scaling factors applied over the 2001 National Emissions Inventory (NEI) are estimated through a four-dimensional variational (4D-Var) approach using SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY) tropospheric NO2 columns measured during summer 2004. In the “top-down” approach, two-month average NO2 columns are assimilated into a regional chemical transport model (CTM), STEM, using different assimilation setups. In a basic setup, NOx emissions are adjusted by assimilating the NO2 columns. A more general setup of emission inversion allows the initial O3 concentrations be adjusted along with the NOx emissions. A final case is set up to assimilate both the NO2 columns and O3 measurement from various platforms while allowing adjustments of both the NOx emissions and the initial O3 concentrations. It is found that the addition of O3 measurements did not improve the NOx emission inversion. With the NOx emission at surface and upper levels being adjusted separately, results from four cases show that the elevated NOx emission reduction ranges from 8.9% to 11.4%, and the surface NOx emission reduction is up to 6.6%. All the cases show NOx emission reduction in Ohio valley and Washington, District of Columbia areas.  相似文献   

16.
EU's programme Clean Air for Europe (CAFE) is presently revising the policy on air quality which will lead to the adoption of a thematic strategy on air pollution under the Sixth Environmental Action Programme by mid-2005. For the abatement of surface ozone it is becoming evident that processes outside European control will be crucial for meeting long-term aims and air quality guidelines in Europe in the future. Measurements and modelling results indicate that there is a strong link between climate change and surface ozone. A warmer and dryer European climate is very likely to lead to increased ozone concentrations. Furthermore, increased anthropogenic emissions in developing economies in Asia are likely to raise the hemispheric background level of ozone. A significant increase in the background concentration of ozone has been observed at several sites in Northern Europe although the underlying causes are not settled. The photochemical formation of tropospheric ozone from increased concentrations of methane and CO may also lead to a higher ozone level on a global scale. Gradually, these effects may outweigh the effect of the reduced European ozone precursor emissions. This calls for a global or hemispheric perspective in the revision of the European air quality policy for ozone.  相似文献   

17.
This study focuses on a new emissions model, Numerical Emissions Model for Air Quality (MNEQA), to be used in photochemical simulations and emission control strategies relating to tropospheric ozone pollutants. MNEQA processes available local information from external files and is easily adaptable to any desired spatial resolution. Top-down and bottom-up methodologies are combined to calculate emissions at the required resolution for photochemical simulations. It was used in conjunction with the MM5-CMAQ air quality modelling system and was applied to an episode of high ozone levels in June 2003. Emission results are widely analysed showing a difference of ?8.8% with EMEP NOx emissions, and ?18.7% with EMEP VOC emissions. Related to ozone simulations, comparative results between measurements and simulations indicated good behaviour of the model in reproducing diurnal ozone concentrations, as statistical values fall within the EPA and EU regulatory frameworks.  相似文献   

18.
The photochemical grid model, UAM-V, has been used by regulatory agencies to make decisions concerning emissions controls, based on studies of the July 1995 ozone episode in the eastern US. The current research concerns the effect of the uncertainties in UAM-V input variables (emissions, initial and boundary conditions, meteorological variables, and chemical reactions) on the uncertainties in UAM-V ozone predictions. Uncertainties of 128 input variables have been estimated and most range from about 20% to a factor of two. 100 Monte Carlo runs, each with new resampled values of each of the 128 input variables, have been made for given sets of median emissions assumptions. Emphasis is on the maximum hourly-averaged ozone concentration during the 12–14 July 1995 period. The distribution function of the 100 Monte Carlo predicted domain-wide maximum ozone concentrations is consistently close to log-normal with a 95% uncertainty range extending over plus and minus a factor of about 1.6 from the median. Uncertainties in ozone predictions are found to be most strongly correlated with uncertainties in the NO2 photolysis rate. Also important are wind speed and direction, relative humidity, cloud cover, and biogenic VOC emissions. Differences in median predicted maximum ozone concentrations for three alternate emissions control assumptions were investigated, with the result that (1) the suggested year-2007 emissions changes would likely be effective in reducing concentrations from those for the year-1995 actual emissions, that (2) an additional 50% NOx emissions reductions would likely be effective in further reducing concentrations, and that (3) an additional 50% VOC emission reductions may not be effective in further reducing concentrations.  相似文献   

19.
ABSTRACT

This paper analyzes the benefits and costs of policies to reduce NOx emissions from electricity generation in the United States. Because emissions of NOx contribute to the high concentration of atmospheric ozone in the eastern states associated with health hazards, the U.S. Environmental Protection Agency (EPA) has called on eastern states to formulate state implementation plans (SIPs) for reducing NOx emissions. Our analysis considers three NOx reduction scenarios: a summer seasonal cap in the eastern states covered by EPA's NOx SIP Call, an annual cap in the same SIP Call region, and a national annual cap. All scenarios allow for emissions trading. Although EPA's current policy is to implement a seasonal cap in the SIP Call region, this analysis indicates that an annual cap in the SIP Call region would yield about $400 million more in net benefits (benefits less costs) than would a seasonal policy, based on particulate-related health effects only. An annual cap in the SIP Call region is also the policy that is most likely to achieve benefits in excess of costs. Consideration of omissions from this accounting, including the potential benefits from reductions in ozone concentrations, strengthens the finding that an annual program offers greater net benefits than does a seasonal program.  相似文献   

20.
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   

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