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1.
Air quality models are used to predict changes in pollutant concentrations resulting from envisioned emission control policies. Recognizing the need to assess the credibility of air quality models in a policy-relevant context, we perform a dynamic evaluation of the Community Multiscale Air Quality (CMAQ) modeling system for the “weekend ozone effect” to determine if observed changes in ozone due to weekday-to-weekend (WDWE) reductions in precursor emissions can be accurately simulated. The weekend ozone effect offers a unique opportunity for dynamic evaluation, as it is a widely documented phenomenon that has persisted since the 1970s. In many urban areas of the Unites States, higher ozone has been observed on weekends than weekdays, despite dramatically reduced emissions of ozone precursors (nitrogen oxides [NOx] and volatile organic compounds [VOCs]) on weekends. More recent measurements, however, suggest shifts in the spatial extent or reductions in WDWE ozone differences. Using 18 years (1988–2005) of observed and modeled ozone and temperature data across the northeastern United States, we re-examine the long-term trends in the weekend effect and confounding factors that may be complicating the interpretation of this trend and explore whether CMAQ can replicate the temporal features of the observed weekend effect. The amplitudes of the weekly ozone cycle have decreased during the 18-year period in our study domain, but the year-to-year variability in weekend minus weekday (WEWD) ozone amplitudes is quite large. Inter-annual variability in meteorology appears to influence WEWD differences in ozone, as well as WEWD differences in VOC and NOx emissions. Because of the large inter-annual variability, modeling strategies using a single episode lasting a few days or a few episodes in a given year may not capture the WEWD signal that exists over longer time periods. The CMAQ model showed skill in predicting the absolute values of ozone concentrations during the daytime. However, early morning NOx concentrations were underestimated and ozone levels were overestimated. Also, the modeled response of ozone to WEWD differences in emissions was somewhat less than that observed. This study reveals that model performance may be improved by (1) properly estimating mobile source NOx emissions and their temporal distributions, especially for diesel vehicles; (2) reducing the grid cell size in the lowest layer of CMAQ; and, (3) using time-dependent and more realistic boundary conditions for the CMAQ simulations.  相似文献   

2.
The advantages and disadvantages, benefits and limitations, of a number of published mathematical models representing the effects of ozone on crops and native vegetation are described. Several levels of modeling are addressed: word models, graphic models, mathematical models, and computer simulation implementation. Special attention is given to evaluating: (1) how the interaction between ozone exposure and vegetation effects is quantified, (2) the status of field testing of the model, and (3) the adequacy of information for enabling other investigators to replicate the model for further testing. Original contributions, not previously published, are made in this evaluation in the form of: (1) graphic model flow charts for published models, (2) clarification of mathematical equations for existing models, (3) graphic forms of functional relations comprising portions of models, and (4) graphic displays of model output performance versus observed data. The models that are evaluated cover acute exposure-response models, statistical and mechanistic-process models, including a partial model of ambient exposure versus ozone flux, and uptake. They also cover chronic exposure statistical approaches, including time-series modeling, mechanistic-process models, 'disintegrated' models of forest system simulations, chronic flux density-uptake-response, and models for regional effects assessment in forests and agricultural lands.  相似文献   

3.
In this paper, the concept of scale analysis is applied to evaluate ozone predictions from two regional-scale air quality models. To this end, seasonal time series of observations and predictions from the RAMS3b/UAM-V and MM5/MAQSIP (SMRAQ) modeling systems for ozone were spectrally decomposed into fluctuations operating on the intra-day, diurnal, synoptic and longer-term time scales. Traditional model evaluation statistics are also presented to illustrate how the scale analysis approach can help improve our understanding of the models’ performance. The results indicate that UAM-V underestimates the total variance (energy) of the ozone time series when compared with observations, but shows a higher mean value than the observations. On the other hand, MAQSIP is able to better reproduce the average energy and mean concentration of the observations. However, both modeling systems do not capture the amount of variability present on the intra-day time scale primarily due to the grid resolution used in the models. For both modeling systems, the correlations between the predictions and observations are insignificant for the intra-day component, high for the diurnal component because of the inherent diurnal cycle but low for the amplitude of the diurnal component, and highest for the synoptic and baseline components. This better model performance on longer time scales suggests that current regional-scale models are most skillful in characterizing average patterns over extended periods, rather than in predicting concentrations at specific locations, during 1–2 day episodic events. In addition, we discuss the implications of these results to using the model-predicted daily maximum ozone concentrations in the regulatory framework in light of the uncertainties introduced by the models’ poor performance on the intra-day and diurnal time scales.  相似文献   

4.
Photochemical grid models are addressing an increasing variety of air quality related issues, yet procedures and metrics used to evaluate their performance remain inconsistent. This impacts the ability to place results in quantitative context relative to other models and applications, and to inform the user and affected community of model uncertainties and weaknesses. More consistent evaluations can serve to drive improvements in the modeling process as major weaknesses are identified and addressed. The large number of North American photochemical modeling studies published in the peer-reviewed literature over the past decade affords a rich data set from which to update previously established quantitative performance “benchmarks” for ozone and particulate matter (PM) concentrations. Here we exploit this information to develop new ozone and PM benchmarks (goals and criteria) for three well-established statistical metrics over spatial scales ranging from urban to regional and over temporal scales ranging from episodic to seasonal. We also recommend additional evaluation procedures, statistical metrics, and graphical methods for good practice. While we primarily address modeling and regulatory settings in the United States, these recommendations are relevant to any such applications of state-of-the-science photochemical models. Our primary objective is to promote quantitatively consistent evaluations across different applications, scales, models, model inputs, and configurations. The purpose of benchmarks is to understand how good or poor the results are relative to historical model applications of similar nature and to guide model performance improvements prior to using results for policy assessments. To that end, it also remains critical to evaluate all aspects of the model via diagnostic and dynamic methods. A second objective is to establish a means to assess model performance changes in the future. Statistical metrics and benchmarks need to be revisited periodically as model performance and the characteristics of air quality change in the future.

Implications: We address inconsistent procedures and metrics used to evaluate photochemical model performance, recommend a specific set of statistical metrics, and develop updated quantitative performance benchmarks for those metrics. We promote quantitatively consistent evaluations across different applications, scales, models, inputs, and configurations, thereby (1) improving the user’s ability to quantitatively place results in context and guide model improvements, and (2) better informing users, regulators, and stakeholders of model uncertainties and weaknesses prior to using results for policy assessments. While we primarily address U.S. modeling and regulatory settings, these recommendations are relevant to any such applications of state-of-the-science photochemical models.  相似文献   


5.
Abstract

In the United States, emission processing models such as Emissions Modeling System-2001 (EMS-2001), Emissions Preprocessor System-Version 2.5 (EPS2.5), and the Sparse Matrix Operator Kernel Emissions (SMOKE) model are currently being used to generate gridded, hourly, speciated emission inputs for urban and regional-scale photochemical models from aggregated pollutant inventories. In this study, two models, EMS-2001 and SMOKE, were applied with their default internal data sets to process a common inventory database for a high ozone (O3) episode over the eastern United States using the Carbon Bond IV (CB4) chemical speciation mechanism. A comparison of the emissions processed by these systems shows differences in all three of the major processing steps performed by the two models (i.e., in temporal allocation, spatial allocation, and chemical speciation). Results from a simulation with a photochemical model using these two sets of emissions indicate differences on the order of ±20 ppb in the predicted 1-hr daily maximum O3 concentrations. It is therefore critical to develop and implement more common and synchronized temporal, spatial, and speciation cross-reference systems such that the processes within each emissions model converge toward reasonably similar results. This would also help to increase confidence in the validity of photochemical grid model results by reducing one aspect of modeling uncertainty.  相似文献   

6.
In the United States, emission processing models such as Emissions Modeling System-2001 (EMS-2001), Emissions Preprocessor System-Version 2.5 (EPS2.5), and the Sparse Matrix Operator Kernel Emissions (SMOKE) model are currently being used to generate gridded, hourly, speciated emission inputs for urban and regional-scale photochemical models from aggregated pollutant inventories. In this study, two models, EMS-2001 and SMOKE, were applied with their default internal data sets to process a common inventory database for a high ozone (O3) episode over the eastern United States using the Carbon Bond IV (CB4) chemical speciation mechanism. A comparison of the emissions processed by these systems shows differences in all three of the major processing steps performed by the two models (i.e., in temporal allocation, spatial allocation, and chemical speciation). Results from a simulation with a photochemical model using these two sets of emissions indicate differences on the order of +/- 20 ppb in the predicted 1-hr daily maximum O3 concentrations. It is therefore critical to develop and implement more common and synchronized temporal, spatial, and speciation cross-reference systems such that the processes within each emissions model converge toward reasonably similar results. This would also help to increase confidence in the validity of photochemical grid model results by reducing one aspect of modeling uncertainty.  相似文献   

7.
This article describes two statistical methods that enable air pollution control agencies to assess the effectiveness of the spatial distribution of current stationary ozone monitoring networks by providing measures of site redundancy. These methods analyze site redundancy by determining the degree to which ozone measurements at one site can be successfully predicted from data collected at other monitoring sites. The first method, the similarity (SIM) measure, calculates redundancy based on the percentage of common operational days during which two monitoring stations report similar daily maximum ozone concentrations. The second method, a modeling technique, relates site redundancy in ozone measurement to an R-squared statistic from an autoregressive model. The model uses meteorological components recorded at a central location and ozone concentrations reported by the network’s other monitoring stations. Both techniques can assist in effective allocation of limited monitoring resources and offer a statistical approach to ambient air monitoring network design. The techniques are applied to data collected at six ozone monitoring stations in Harris County, Texas, during an eight-year period in the 1980s. The methods identified two sites in the six-site network that exhibit a high degree of redundancy.  相似文献   

8.
The U.S. Environmental Protection Agency provides guidelines for demonstrating that future 8-hr ozone (O3) design values will be at or below the National Ambient Air Quality Standards on the basis of the application of photochemical modeling systems to simulate the effect of emission reductions. These guidelines also require assessment of the model simulation against observations. In this study, we examined the link between the simulated relative responses to emission reductions and model performance as measured by operational evaluation metrics, a part of the model evaluation required by the guidance, which often is the cornerstone of model evaluation in many practical applications. To this end, summertime O3 concentrations were simulated with two modeling systems for both 2002 and 2009 emission conditions. One of these two modeling systems was applied with two different parameterizations for vertical mixing. Comparison of the simulated base-case 8-hr daily maximum O3 concentrations showed marked model-to-model differences of up to 20 ppb, resulting in significant differences in operational model performance measures. In contrast, only relatively minor differences were detected in the relative response of O3 concentrations to emission reductions, resulting in differences of a few ppb or less in estimated future year design values. These findings imply that operational model evaluation metrics provide little insight into the reliability of the actual model application in the regulatory setting (i.e., the estimation of relative changes). In agreement with the guidance, it is argued that more emphasis should be placed on the diagnostic evaluation of O3-precursor relationships and on the development and application of dynamic and retrospective evaluation approaches in which the response of the model to changes in meteorology and emissions is compared with observed changes. As an example, simulated relative O3 changes between 1995 and 2007 are compared against observed changes. It is suggested that such retrospective studies can serve as the starting point for targeted diagnostic studies in which individual aspects of the modeling system are evaluated and refined to improve the characterization of observed changes.  相似文献   

9.
ABSTRACT

A predominantly rural ozone monitoring network was operated under the auspices of the Clean Air Status and Trends Network (CASTNet) from 1988 until 1995. Ozone data from sites in the eastern United States are presented and several indices are used to describe the spatial and temporal distribution of ozone concentration and exposure. These indices are SUM06, W126, the 8-hour rolling average (MAX8hr>80), and the current National Ambient Air Quality Standards (NAAQS) for ozone. Ozone indices were selected to illustrate the spatial and temporal distribution of ozone, and the sensitivity of this distribution to different representations of concentration or exposure.

CASTNet is unique in that a uniform set of site selection criteria and uniform procedures, including traceability to a single primary standard, provide a high degree of comparability across sites. Sites were selected to avoid undue influence from point sources, area sources, or local activities. The sites reflect a wide range of land use and terrain types including agricultural and forested, in flat, rolling, and complex terrain from the eastern seaboard across the Appalachian Mountains to the Midwest.

Results indicate that ozone concentrations varied greatly in time and space across the eastern United States. Sites in the upper northeast, upper midwest, and southern periphery subregions experienced relatively low ozone during the years of record compared to sites in the northeast, midwest, and south central subregions. Ozone exposures at an individual rural site are dependent on many factors, including terrain, meteorology, and distance from sources of precursors. Relative to the current (as of 1996) NAAQS, only a handful of CASTNet sites near major urban areas report exceedances. In contrast, the majority of CASTNet sites might exceed the proposed new primary standard for ozone.

Sites at high elevation (>900m) in the east exhibit relatively high exposure statistics (e.g., SUM06 and W126), but no exceedance of the current ozone standard from 1988 through 1995. Terrain effects explain some of the variability within subregions and are an important consideration in the design of monitoring networks for ozone and possibly other pollutants.  相似文献   

10.
A real-time air quality forecasting system (Eta-Community Multiscale Air Quality [CMAQ] model suite) has been developed by linking the National Centers for Environmental Estimation Eta model to the U.S. Environmental Protection Agency (EPA) CMAQ model. This work presents results from the application of the Eta-CMAQ modeling system for forecasting ozone (O3) over the Northeastern United States during the 2002 New England Air Quality Study (NEAQS). Spatial and temporal performance of the Eta-CMAQ model for O3 was evaluated by comparison with observations from the EPA Air Quality System (AQS) network. This study also examines the ability of the model to simulate the processes governing the distributions of tropospheric O3 on the basis of the intensive datasets obtained at the four Atmospheric Investigation, Regional Modeling, Analysis, and Estimation (AIRMAP) and Harvard Forest (HF) surface sites. The episode analysis reveals that the model captured the buildup of O3 concentrations over the northeastern domain from August 11 and reproduced the spatial distributions of observed O3 very well for the daytime (8:00 p.m.) of both August 8 and 12 with most of normalized mean bias (NMB) within +/- 20%. The model reproduced 53.3% of the observed hourly O3 within a factor of 1.5 with NMB of 29.7% and normalized mean error of 46.9% at the 342 AQS sites. The comparison of modeled and observed lidar O3 vertical profiles shows that whereas the model reproduced the observed vertical structure, it tended to overestimate at higher altitude. The model reproduced 64-77% of observed NO2 photolysis rate values within a factor of 1.5 at the AIRMAP sites. At the HF site, comparison of modeled and observed O3/nitrogen oxide (NOx) ratios suggests that the site is mainly under strongly NOx-sensitive conditions (>53%). It was found that the modeled lower limits of the O3 production efficiency values (inferred from O3-CO correlation) are close to the observations.  相似文献   

11.
The objective of this study was to establish whether EU and UN-ECE/ICP-Forests monitoring data (i) provide the variables necessary to apply the flux-based modeling methods and (ii) meet the quality criteria necessary to apply the flux-based critical level concept. Application of this model has been possible using environmental data collected from the EU and UN-ECE/ICP-Forests monitoring network in Switzerland and Italy for 2000-2002. The test for data completeness and plausibility resulted in 6 out of a possible total of 20 Fagus sylvatica L. plots being identified as suitable from Switzerland, Italy, Spain, and France. The results show that the collected data allow the identification of different spatial and temporal areas and periods as having higher risk to ozone than those identified using the AOT40 approach. However, it was also apparent that the quality and completeness of the available data may severely limit a complete risk assessment across Europe.  相似文献   

12.
Ozone is a widely distributed pollutant in the atmospheric boundary layer over north west Europe. Three main sources have been identified: the stratosphere, the free troposphere and boundary layer photochemical production. The pattern of ground level ozone concentrations resulting from these three sources cannot be accurately specified. Ozone shows significant variations in space and time but because of the high cost of continuous monitoring equipment, spatial variations on a national and international basis have not been studied in detail. Variations in ozone concentrations at individual monitoring sites have been given a great deal of attention and experience gained from United Kingdom monitoring sites is described in some detail. The averaging time statistical model of Larsen is employed to relate the exposure levels measured over different averaging periods. Diurnal variations have a major influence on exposure levels at sites nominally exposed to the same regional ozone distribution. The physical and chemical mechanisms which give rise to diurnal variations are detailed so that sites can be screened for different diurnal behaviour characteristics.  相似文献   

13.
A Bayesian hierarchical regime switching model describing the spatial–temporal behavior of ozone (O3) within a domain covering Lake Michigan during spring–summer 1999 is developed. The model incorporates linkages between ozone and meteorology. It is specifically formulated to identify meteorological regimes conducive of high ozone levels and allow ozone behavior during these periods to be different from typical ozone behavior. The model is used to estimate or forecast spatial fields of O3 conditional on observed (or forecasted) meteorology including temperature, humidity, pressure, and wind speed and direction. The model is successful at forecasting the onset of periods of high ozone levels, but more work is needed to also accurately identify departures from these periods.  相似文献   

14.
Cross-border transport of ozone is one of the most contentious issues of air pollution management in the U.S. Yet, both the modeling and observational studies are lacking. Models are normally validated by comparing predicted and observed ozone concentrations. However, proper validation of cross-border transport model requires a comparison of predictions against observation-based benchmarks of cross-border ozone transport. Such benchmarks are unavailable, as published observation-based studies always deal only with a combination of local production and cross-border transport, not a cross-border transport itself. We show how to extract necessary benchmarks from observations of rural monitoring sites near state borders. On example of the western border of New York, we find that in about two-thirds of the most polluted days all the ozone came in a steady cross-border inflow after previously passing over one or more large urban areas to the west. In all the enumerated days with direct cross-border inflow, daily maximum 8-hr concentrations of ozone just upwind of the border were over 60 ppb, with an average value of 68 ppb, just short of the 70 ppb ozone regulatory threshold, information also useful to state air pollution authorities.

Implications: The purpose of the cross-border ozone pollution models is to predict cross-border transport of ozone, so the ability of the model to accurately represent observed ozone concentrations is necessary but not sufficient for model validation. The accuracy of predicted ozone concentrations is not necessarily the same as the accuracy of the predictions of ozone transport. Proper model validation requires comparisons against observation-based benchmarks of cross-border transport. Such observations, so far absent, can be obtained from rural monitoring sites near state borders, as illustrated by the example of western New York.  相似文献   


15.
16.
ABSTRACT

A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas.

The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.  相似文献   

17.
A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas. The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.  相似文献   

18.
Large petrochemical flares, common in the Houston Ship Channel (the Ship Channel) and other industrialized areas in the Gulf of Mexico region, emit hundreds to thousands of pounds per hour of highly reactive volatile organic compounds (HRVOCs). We employed fine horizontal resolution (200 m?×?200 m) in a three-dimensional (3D) Eulerian chemical transport model to simulate two historical Ship Channel flares. The model reasonably reproduced the observed ozone rise at the nearest monitoring stations downwind of the flares. The larger of the two flares had an olefin emission rate exceeding 1400 lb/hr. In this case, the model simulated a rate of increase in peak ozone greater than 40 ppb/hr over a 12 km?×?12 km horizontal domain without any unusual meteorological conditions. In this larger flare, formaldehyde emissions typically neglected in official inventories enhanced peak ozone by as much as 16 ppb and contributed over 10 ppb to ambient formaldehyde up to ~8 km downwind of the flare. The intense horizontal gradients in large flare plumes cannot be simulated by coarse models typically used to demonstrate ozone attainment. Moreover, even the relatively dense monitoring network in the Ship Channel may not be able to detect many transient high ozone events (THOEs) caused by industrial flare emissions in the absence of stagnant air recirculation or stalled sea breeze fronts, even though such conditions are unnecessary for the occurrence of THOEs.

Implications: Flare minimization may be an important strategy to attain the U.S. federal ozone standard in industrialized areas, and to avoid inordinate exposure to formaldehyde in neighborhoods surrounding petrochemical facilities. Moreover, air quality monitoring networks, emission inventories, and chemical transport models with higher spatial and temporal resolution and more refined speciation of HRVOCs are needed to better account for the near-source air quality impacts of large olefin flares.  相似文献   

19.
Abstract

A real-time air quality forecasting system (Eta-Community Multiscale Air Quality [CMAQ] model suite) has been developed by linking the National Centers for Environmental Estimation Eta model to the U.S. Environmental Protection Agency (EPA) CMAQ model. This work presents results from the application of the Eta-CMAQ modeling system for forecasting ozone (O3) over the Northeastern United States during the 2002 New England Air Quality Study (NEAQS). Spatial and temporal performance of the Eta-CMAQ model for O3 was evaluated by comparison with observations from the EPA Air Quality System (AQS) network. This study also examines the ability of the model to simulate the processes governing the distributions of tropospheric O3 on the basis of the intensive datasets obtained at the four Atmospheric Investigation, Regional Modeling, Analysis, and Estimation (AIRMAP) and Harvard Forest (HF) surface sites. The episode analysis reveals that the model captured the buildup of O3 concentrations over the northeastern domain from August 11 and reproduced the spatial distributions of observed O3 very well for the daytime (8:00 p.m.) of both August 8 and 12 with most of normalized mean bias (NMB) within [H11006]20%. The model reproduced 53.3% of the observed hourly O3 within a factor of 1.5 with NMB of 29.7% and normalized mean error of 46.9% at the 342 AQS sites.The comparison of modeled and observed lidar O3 vertical profiles shows that whereas the model reproduced the observed vertical structure, it tended to overestimate at higher altitude. The model reproduced 64 –77% of observed NO2 photolysis rate values within a factor of 1.5 at the AIRMAP sites. At the HF site, comparison of modeled and observed O3/nitrogen oxide (NOx) ratios suggests that the site is mainly under strongly NOx-sensitive conditions (>53%). It was found that the modeled lower limits of the O3 production efficiency values (inferred from O3-CO correlation) are close to the observations.  相似文献   

20.
Stochastic models that estimate the ground-level ozone concentrations in air at an urban and rural sampling points in South-eastern Spain have been developed. Studies of temporal series of data, spectral analyses of temporal series and ARIMA models have been used. The ARIMA model (1,0,0) x (1,0,1)24 satisfactorily predicts hourly ozone concentrations in the urban area. The ARIMA (2,1,1) x (0,1,1)24 has been developed for the rural area. In both sampling points, predictions of hourly ozone concentrations agree reasonably well with measured values. However, the prediction of hourly ozone concentrations in the rural point appears to be better than that of the urban point. The performance of ARIMA models suggests that this kind of modelling can be suitable for ozone concentrations forecasting.  相似文献   

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