An Assessment of the Emissions Inventory Processing Systems EMS-2001 and SMOKE in Grid-Based Air Quality Models

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.     

Parameter Evaluation and Model Validation of Ozone Exposure Assessment Using Harvard Southern California Chronic Ozone Exposure Study Data

Abstract

To examine factors influencing long‐term ozone (O₃) exposures by children living in urban communities, the authors analyzed longitudinal data on personal, indoor, and outdoor O₃ concentrations, as well as related housing and other questionnaire information collected in the one‐year‐long Harvard Southern California Chronic Ozone Exposure Study. Of 224 children contained in the original data set, 160 children were found to have longitudinal measurements of O₃ concentrations in at least six months of 12 months of the study period. Data for these children were randomly split into two equal sets: one for model development and the other for model validation. Mixed models with various variance‐covariance structures were developed to evaluate statistically important predictors for chronic personal ozone exposures. Model predictions were then validated against the field measurements using an empirical best‐linear unbiased prediction technique.The results of model fitting showed that the most important predictors for personal ozone exposure include indoor O₃ concentration, central ambient O₃ concentration, outdoor O₃ concentration, season, gender, outdoor time, house fan usage, and the presence of a gas range in the house. Hierarchical models of personal O₃ concentrations indicate the following levels of explanatory power for each of the predictive models: indoor and outdoor O₃ concentrations plus questionnaire variables, central and indoor O₃ concentrations plus questionnaire variables, indoor O₃ concentrations plus questionnaire variables, central O₃ concentrations plus questionnaire variables, and questionnaire data alone on time activity and housing characteristics. These results provide important information on key predictors of chronic human exposures to ambient O₃ for children and offer insights into how to reliably and cost‐effectively predict personal O₃ exposures in the future. Furthermore, the techniques and findings derived from this study also have strong implications for selecting the most reliable and cost‐effective exposure study design and modeling approaches for other ambient pollutants, such as fine particulate matter and selected urban air toxics.     

A land use regression for predicting fine particulate matter concentrations in the New York City region

We developed regression equations to predict fine particulate matter (PM_2.5) at air monitoring locations in the New York City region using data on nearby traffic and land use patterns. Three-year averages (1999–2001) of PM_2.5 at US Environmental Protection Agency (EPA) monitors in the 28 counties including and surrounding New York City were calculated using daily data from the EPA's Air Quality Subsystem. As the secondary contribution to PM_2.5 concentrations is lowest in the winter, we also calculated and modeled average winter 2000 PM_2.5 to conduct a preliminary evaluation of model sensitivity to source contribution. Candidate predictor variables included traffic, land use, census and emissions data from local, state and national sources and were tabulated for a series of circular buffer regions at varying distances around the monitors using a geographic information system. In total, more than 25 variables at 5 different buffer distances were considered for inclusion in the model. Before evaluating the variables we removed several samples from the modeling for validation. For comparison and validation purposes we computed both a model using data for the full 28-county region as well as a more urbanized 9-county region. We found that traffic within a buffer of 300 or 500 m explains the greatest proportion of variance (37–44%) in all 3 models. Measures of urbanization, specifically population density, explain a significant amount of the residual variation (7–18%) after including a traffic variable. Finally, a measure of industrial land use further improves the 28-county and 9-county models based on the 3-yr annual averages, explaining an additional 4% and 11% of the variation, respectively, while vegetative land use improves the winter model explaining an additional 6%. The final models predicted well at validation locations. In total, the final land use regression models explain between 61% and 64% of the variation in PM_2.5.     

Testing the Potential for Predictive Modeling and Mapping and Extending Its Use as a Tool for Evaluating Management Scenarios and Economic Valuation in the Baltic Sea (PREHAB)

We evaluated performance of species distribution models for predictive mapping, and how models can be used to integrate human pressures into ecological and economic assessments. A selection of 77 biological variables (species, groups of species, and measures of biodiversity) across the Baltic Sea were modeled. Differences among methods, areas, predictor, and response variables were evaluated. Several methods successfully predicted abundance and occurrence of vegetation, invertebrates, fish, and functional aspects of biodiversity. Depth and substrate were among the most important predictors. Models incorporating water clarity were used to predict increasing cover of the brown alga bladderwrack Fucus vesiculosus and increasing reproduction area of perch Perca fluviatilis, but decreasing reproduction areas for pikeperch Sander lucioperca following successful implementation of the Baltic Sea Action Plan. Despite variability in estimated non-market benefits among countries, such changes were highly valued by citizens in the three Baltic countries investigated. We conclude that predictive models are powerful and useful tools for science-based management of the Baltic Sea.     

Analysis of air pollution data at a mixed source location using boosted regression trees

This paper explores the use of boosted regression trees to draw inferences concerning the source characteristics at a location of high source complexity. Models are developed for hourly concentrations of nitrogen oxides (NO_X) close to a large international airport. Model development is discussed and methods to quantify model uncertainties developed. It is shown that good explanatory models can be developed and further, allowing for interactions between model variables significantly improves the model fits compared with non-interacting models. Methods are used to determine which variables exert most influence over predicted concentrations and to explore the NO_X dependency for each. Model predictions are used to estimate aircraft take-off contributions to total concentrations of NO_X and determine how these predictions are affected by annual variations in meteorological conditions and runway use patterns. Furthermore, the results relating to the aircraft contributions to total NO_X concentration are compared with those from a more detailed independent field campaign. Finally, we find empirical evidence that plumes from larger aircraft disperse more rapidly from the point of release compared with smaller aircraft. The reasons for this behaviour and the implications are discussed.     

Development of Models for Predicting the Distribution of Indoor Nitrogen Dioxide Concentrations

Extensive data on residential indoor and outdoor NO₂ levels have been collected in a limited number of U.S. locations. To date, researchers have analyzed these data sets individually, but have not analyzed them in the aggregate. Results have not, therefore, been suitable for application in a nationwide exposure assessment. This paper presents an analysis of indoor and outdoor NO₂ field measurements from five U.S. metropolitan areas for homes with gas-fueled ranges and discusses potential applications of the results. Using linear regression analysis, the relationship between indoor NO₂ and various predictor variables was explored. Results indicated that ambient NO2 levels alone explain an estimated 37 percent of the variability in indoor NO₂ levels, that the relationship between indoor and outdoor NO₂ concentrations differs significantly from summer to winter months, and that homes with range pilot lights have indoor levels approximately 7 ppb greater than homes without pilot lights. A logistic regression model which predicts the distribution of indoor NO₂ levels based on ambient NO₂ concentrations was developed. Estimation and testing of the logistic model indicated good model performance. The model is particularly useful for addressing policy-oriented questions that involve the concept of "acceptable" threshold levels for human exposure to NO₂.     

Validation of Personal Exposure Models for Sulfafe and Aerosol Strong Acidity

Personal exposure models for sulfates (SO₄ ⁼) and aerosol strong acidity (H⁺) were previously developed using concentration and activity pattern data collected from a personal monitoring study conducted in Uniontown, Pennsylvania, during the summer of 1990. Models were constructed based on time-weighted microenvironmental exposures. For SO₄ ⁼, the “best-fit” model included a correction factor, while for H⁺, it included both a correction factor and a neutralization term.

In this paper, we present the validation of these models using data collected in a personal monitoring study conducted in State College, Pennsylvania, during the summer of 1991. Indoor and outdoor concentration and activity pattern data collected in this study were used as inputs for the “best-fit” models for SO₄ ⁼ and H⁺. Predicted personal exposures subsequently were compared to the measured personal exposures from State College to determine their accuracy and precision.

Predicted personal exposures for both SO₄ ⁼ and H⁺ were in excellent agreement with measured personal exposures from State College. The models explained 91 and 62 percent of the variability in personal SO₄ ⁼ and H⁺ exposures, respectively, and were able to estimate personal exposures substantially better than outdoor concentrations alone. Validation results suggest that the models' correction and neutralization factors are not site specific and support the models' future application as a technique to assess the personal acid aerosol exposures of children living in similar rural and semi-rural communities.     

Impacts of Meteorological Factors on PM10: Artificial Neural Networks (ANN) and Multiple Linear Regression (MLR) Approaches

In this study, prediction capacities of multi-linear regression (MLR) and artificial neural networks (ANN) onto coarse particulate matter (PM₁₀) concentrations were investigated. Different meteorological factors on particulate pollution were chosen for operating variables in the model analyses. Two different regions (urban and industrial) were identified in the region of Kocaeli, Turkey. All data sets were obtained from air quality monitoring network of the Ministry of Environment and Urban Planning, and 120 data sets were used in the MLR and ANN models. Regression equations explained the effects of the meteorological factors in MLR analyses. In the ANN model, backpropagation network with two hidden layers has achieved the best prediction efficiency. Determination coefficients and error values were examined for each model. ANN models displayed more accurate results compared to MLR.     

Optimization of artificial neural network models through genetic algorithms for surface ozone concentration forecasting

Introduction

This study proposes three methodologies to define artificial neural network models through genetic algorithms (GAs) to predict the next-day hourly average surface ozone (O₃) concentrations. GAs were applied to define the activation function in hidden layer and the number of hidden neurons.

Methods

Two of the methodologies define threshold models, which assume that the behaviour of the dependent variable (O₃ concentrations) changes when it enters in a different regime (two and four regimes were considered in this study). The change from one regime to another depends on a specific value (threshold value) of an explanatory variable (threshold variable), which is also defined by GAs. The predictor variables were the hourly average concentrations of carbon monoxide (CO), nitrogen oxide, nitrogen dioxide (NO₂), and O₃ (recorded in the previous day at an urban site with traffic influence) and also meteorological data (hourly averages of temperature, solar radiation, relative humidity and wind speed). The study was performed for the period from May to August 2004.

Results and discussion

Several models were achieved and only the best model of each methodology was analysed. In threshold models, the variables selected by GAs to define the O₃ regimes were temperature, CO and NO₂ concentrations, due to their importance in O₃ chemistry in an urban atmosphere.

Conclusion

In the prediction of O₃ concentrations, the threshold model that considers two regimes was the one that fitted the data most efficiently.     

Stochastic simulation of meteorological variability for long-range atmospheric transport—II. Long-term statistical models

Methods are developed for simulating meteorological inputs for statistical atmospheric transport models. Stochastic models are presented for the annual mean wind vector, the horizontal diffusion coefficient, the fraction of time it is raining, and the quantity of precipitation. The models are derived by aggregating the statistical models for short-term meteorological processes given in the companion paper of Small and Samson (Atmospheric Environment, 1989, 23, 2813–2824). Normal distributions are used for each variable. The normal distribution is derived directly for the mean wind vector based on the normality of short-term winds, and serves as an acceptable approximation for the other variables given their low interannual coefficient of variation. Correlation between variables is considered, including correlation between winds and precipitation, between the fraction of time it is raining and the total quantity of precipitation at a site, and between the annual precipitation quantity at multiple sites. Development and confirmation of the interannual distributions is supported by long-term meteorological data, including a nine-year backward trajectory record computed for a site in western Pennsylvania. Application of the method is demonstrated with a statistical atmospheric LRT model used to predict distributions of annual precipitation sulfates in eastern North America. Predicted interannual coefficients of variation of wet SO₄²⁻ concentrations range from about 10 to 15 per cent, similar to the level of interannual variation inferred from long-term data sets.     

Bulgarian emergency response models–validation against ETEX first release

In the paper, the performance of two Bulgarian dispersion models is tested against European Tracer Experiment (ETEX) first release data base. The first one is the LED puff model which was the core of the Bulgarian Emergency Response System during all releases of ETEX. The second one is the newly created Eulerian dispersion model EMAP. These models have two important features: they are PC-oriented and they use quite a limited amount of input meteorological information. First, a number of runs with various source configurations are made on meteorological data produced by ECMWF. The aim of these runs is to verify the models’ ability to simulate reliably ETEX first release. To this end, a set of statistical criteria selected in ATMES (Atmospheric Transport Models Evaluation Study, see Klug et al., 1992 are used. The best runs for both models are obtained when the source is presented as a column towering from the ground to heights of 400–700 m. These runs took part in the second phase of ETEX (ETEX-II), the so called ATMES-type exercise where EMAP ranked ninth and LED - fourteenth among 34 models. Here, additional sets of EMAP are presented where in the first run the value of the horizontal diffusion coefficient is varied and in the other runs different meteorological data sets are tested. The results obtained from the first run show that the values of K_h=4–6×10⁴ m² s^-1 produce fields which fit experimental data best. The other sets of runs show that the higher the frequency of the meteorological data, the better the simulation. The results can be improved by linear interpolation of the meteorological parameters with time, the best fitting obtained with interpolation at each time step.     

A Comparative Validation of the RAM and PTMTP Models for Short-Term SO2 Concentrations in Two Urban Areas

A comprehensive and comparative model validation of two EPA models for short-term SO₂ concentrations was performed. The two models tested were RAM (Urban version) and PTMTP (Terrain version). Both are multiple source, multiple receptor gaussian plume models, recommended in the EPA Guideline On Air Quality Models. ¹ The principal difference between the two models is in their use of empirical dispersion coefficients. It was because of the potential for markedly different predicted maximum SO₂ concentrations, and the absence of any testing data on the RAM model, that the validation analysis was undertaken. The current study utilized a full year of air quality data from monitoring sites in two Indiana cities, Michigan City and Indianapolis. Cumulative frequency distributions for each site and model were prepared and comparisons made. The results indicate that the RAM (Urban) model was highly inaccurate in predicting maximum short-term SO₂ concentrations. The PTMTP model, although conservative in its estimates, produces results which more closely resemble the distribution of observed SO₂ concentrations. The body of information presented in this paper is directed to environmental scientists responsible for air quality modeling, and to those persons who set policy on the use of models in air quality studies.     

Predicting hourly air pollutant levels using artificial neural networks coupled with uncertainty analysis by Monte Carlo simulations

Recent progress in developing artificial neural network (ANN) metamodels has paved the way for reliable use of these models in the prediction of air pollutant concentrations in urban atmosphere. However, improvement of prediction performance, proper selection of input parameters and model architecture, and quantification of model uncertainties remain key challenges to their practical use. This study has three main objectives: to select an ensemble of input parameters for ANN metamodels consisting of meteorological variables that are predictable by conventional weather forecast models and variables that properly describe the complex nature of pollutant source conditions in a major city, to optimize the ANN models to achieve the most accurate hourly prediction for a case study (city of Tehran), and to examine a methodology to analyze uncertainties based on ANN and Monte Carlo simulations (MCS). In the current study, the ANNs were constructed to predict criteria pollutants of nitrogen oxides (NO_x), nitrogen dioxide (NO₂), nitrogen monoxide (NO), ozone (O₃), carbon monoxide (CO), and particulate matter with aerodynamic diameter of less than 10 μm (PM₁₀) in Tehran based on the data collected at a monitoring station in the densely populated central area of the city. The best combination of input variables was comprehensively investigated taking into account the predictability of meteorological input variables and the study of model performance, correlation coefficients, and spectral analysis. Among numerous meteorological variables, wind speed, air temperature, relative humidity and wind direction were chosen as input variables for the ANN models. The complex nature of pollutant source conditions was reflected through the use of hour of the day and month of the year as input variables and the development of different models for each day of the week. After that, ANN models were constructed and validated, and a methodology of computing prediction intervals (PI) and probability of exceeding air quality thresholds was developed by combining ANNs and MCSs based on Latin Hypercube Sampling (LHS). The results showed that proper ANN models can be used as reliable metamodels for the prediction of hourly air pollutants in urban environments. High correlations were obtained with R ² of more than 0.82 between modeled and observed hourly pollutant levels for CO, NO_x, NO₂, NO, and PM₁₀. However, predicted O₃ levels were less accurate. The combined use of ANNs and MCSs seems very promising in analyzing air pollution prediction uncertainties. Replacing deterministic predictions with probabilistic PIs can enhance the reliability of ANN models and provide a means of quantifying prediction uncertainties.     

Estimated long-term outdoor air pollution concentrations in a cohort study

Several recent studies associated long-term exposure to air pollution with increased mortality. An ongoing cohort study, the Netherlands Cohort Study on Diet and Cancer (NLCS), was used to study the association between long-term exposure to traffic-related air pollution and mortality. Following on a previous exposure assessment study in the NLCS, we improved the exposure assessment methods.Long-term exposure to nitrogen dioxide (NO₂), nitrogen oxide (NO), black smoke (BS), and sulphur dioxide (SO₂) was estimated. Exposure at each home address (N=21 868) was considered as a function of a regional, an urban and a local component. The regional component was estimated using inverse distance weighed interpolation of measurement data from regional background sites in a national monitoring network. Regression models with urban concentrations as dependent variables, and number of inhabitants in different buffers and land use variables, derived with a Geographic Information System (GIS), as predictor variables were used to estimate the urban component. The local component was assessed using a GIS and a digital road network with linked traffic intensities. Traffic intensity on the nearest road and on the nearest major road, and the sum of traffic intensity in a buffer of 100 m around each home address were assessed. Further, a quantitative estimate of the local component was estimated.The regression models to estimate the urban component explained 67%, 46%, 49% and 35% of the variances of NO₂, NO, BS, and SO₂ concentrations, respectively. Overall regression models which incorporated the regional, urban and local component explained 84%, 44%, 59% and 56% of the variability in concentrations for NO₂, NO, BS and SO₂, respectively.We were able to develop an exposure assessment model using GIS methods and traffic intensities that explained a large part of the variations in outdoor air pollution concentrations.     

Application of air pollution dispersion modeling for source-contribution assessment and model performance evaluation at integrated industrial estate-Pantnagar

Source-contribution assessment of ambient NO₂ concentration was performed at Pantnagar, India through simulation of two urban mathematical dispersive models namely Gaussian Finite Line Source Model (GFLSM) and Industrial Source Complex Model (ISCST-3) and model performances were evaluated. Principal approaches were development of comprehensive emission inventory, monitoring of traffic density and regional air quality and conclusively simulation of urban dispersive models. Initially, 18 industries were found responsible for emission of 39.11 kg/h of NO₂ through 43 elevated stacks. Further, vehicular emission potential in terms of NO₂ was computed as 7.1 kg/h. Air quality monitoring delineates an annual average NO₂ concentration of 32.6 μg/m³. Finally, GFLSM and ISCST-3 were simulated in conjunction with developed emission inventories and existing meteorological conditions. Models simulation indicated that contribution of NO₂ from industrial and vehicular source was in a range of 45-70% and 9-39%, respectively. Further, statistical analysis revealed satisfactory model performance with an aggregate accuracy of 61.9%.     

A Study of the Association between Daily Mortality and Ambient Air Pollutant Concentrations in Pittsburgh,Pennsylvania

ABSTRACT

We have studied the possible association of daily mortality with ambient pollutant concentrations (PM₁₀, CO, O₃, SO₂, NO₂, and fine [PM_{2 5}] and coarse PM) and weather variables (temperature and dew point) in the Pittsburgh, PA, area for two age groups—less than 75, and 75 and over—for the 3-year period of 1989-1991. Correlation functions among pollutant concentrations show important seasonal dependence, and this fact necessitates the use of seasonal models to better identify the link between ambient pollutant concentrations and daily mortality. An analysis of the seasonal model results for the younger-age group reveals significant multicollinearity problems among the highly correlated concentrations of PM₁₀, CO, and NO₂ (and O₃ in spring and summer), and calls into question the rather consistent results of the single- and multi-pollutant non-seasonal models that show a significant positive association between PM₁₀ and daily mortality. For the older-age group, dew point consistently shows a significant association with daily mortality in all models. Collinearity problems appear in the multi-pollutant seasonal and non-seasonal models such that a significant, positive PM₁₀ coefficient is accompanied by a significant, negative coefficient of another ambient pollutant, and the identity of this other pollutant changes with season. The PM₂₅ data set is half that of PM₁₀. Identical-model runs for both data sets reveal instability in the pollutant coefficients, especially for the younger age group. The concern for the instability of the pollutant coefficients due to a small signal-to-noise ratio makes it impossible to ascertain credibly the relative associations of the fine- and coarse-particle modes with daily mortality. In this connection, we call for caution in the interpretation of model results for causal inference when the models use fully or partially estimated PM values to fill large data gaps.     

Comparison of models used for national agricultural ammonia emission inventories in Europe: Litter-based manure systems

Six N-flow models, used to calculate national ammonia (NH₃) emissions from agriculture in different European countries, were compared using standard data sets. Scenarios for litter-based systems were run separately for beef cattle and for broilers, with three different levels of model standardisation: (a) standardized inputs to all models (FF scenario); (b) standard N excretion, but national values for emission factors (EFs) (FN scenario); (c) national values for N excretion and EFs (NN scenario). Results of the FF scenario for beef cattle produced very similar estimates of total losses of total ammoniacal-N (TAN) (±6% of the mean total), but large differences in NH₃ emissions (±24% of the mean). These differences arose from the different approaches to TAN immobilization in litter, other N losses and mineralization in the models. As a result of those differences estimates of TAN available at spreading differed by a factor of almost 3. Results of the FF scenario for broilers produced a range of estimates of total changes in TAN (±9% of the mean total), and larger differences in the estimate of NH₃ emissions (±17% of the mean). The different approaches among the models to TAN immobilization, other N losses and mineralization, produced estimates of TAN available at spreading which differed by a factor of almost 1.7. The differences in estimates of NH₃ emissions decreased as estimates of immobilization and other N losses increased. Since immobilization and denitrification depend also on the C:N ratio in manure, there would be advantages to include C flows in mass-flow models. This would also provide an integrated model for the estimation of emissions of methane, non-methane VOCs and carbon dioxide. Estimation of these would also enable an estimate of mass loss, calculation of the N and TAN concentrations in litter-based manures and further validation of model outputs.     

A study on the evaluations of emission factors and uncertainty ranges for methane and nitrous oxide from combined-cycle power plant in Korea

In this research, in order to develop technology/country-specific emission factors of methane (CH₄) and nitrous oxide (N₂O), a total of 585 samples from eight gas-fired turbine combined cycle (GTCC) power plants were measured and analyzed. The research found that the emission factor for CH₄ stood at “0.82 kg/TJ”, which was an 18 % lower than the emission factor for liquefied natural gas (LNG) GTCC “1 kg/TJ” presented by Intergovernmental Panel on Climate Change (IPCC). The result was 8 % up when compared with the emission factor of Japan which stands at “0.75 kg/TJ”. The emission factor for N₂O was “0.65 kg/TJ”, which is significantly lower than “3 kg/TJ” of the emission factor for LNG GTCC presented by IPCC, but over six times higher than the default N₂O emission factor of LNG. The evaluation of uncertainty was conducted based on the estimated non-CO₂ emission factors, and the ranges of uncertainty for CH₄ and N₂O were between ?12.96 and +13.89 %, and ?11.43 and +12.86 %, respectively, which is significantly lower than uncertainties presented by IPCC. These differences proved that non-CO₂ emissions can change depending on combustion technologies; therefore, it is vital to establish country/technology-specific emission factors.