Future year ozone source attribution modeling study using CMAQ-ISAM.

To achieve the current United States National Ambient Air Quality Standards (NAAQS) attainment level for ozone or particulate matter, current photochemical air quality models include tools to determine source apportionment and/or source sensitivity. Previous studies by the authors have used the Ozone and Particulate Matter Source Apportionment Technology and Higher-order Decoupled Direct Method probing tools in CAMx to investigate these source-receptor relationships for ozone. The recently available source apportionment for CMAQ, referred to as the Integrated Source Apportionment Method (ISAM), was used in this study to conduct future year (2030) source attribution modeling. The CMAQ-ISAM ozone source attribution results for selected cities across the U.S. showed boundary conditions were the dominant contributor to the future year highest July maximum daily 8-hour average (MDA8) ozone concentrations. Point sources were generally larger contributors in the eastern U.S. than in the western U.S. The contributions of on-road mobile emissions were around 5 ppb at most of the cities selected for analysis. Off-road mobile source contributions were around 20 ppb or nearly 30%. Since boundary conditions play an important role in future year ozone levels, it is important to characterize future year boundary conditions accurately. The current implementation of ISAM in CMAQ 5.0.2 requires significant computing resources for ozone source attribution, making it difficult to conduct long-term simulations for large domains. The computing requirements for PM source attribution are even more onerous. CMAQ 5.2 was released after this study was completed, and does not include ISAM. If an efficient version of ISAM becomes available, it could be used in long-term ozone and PM2.5 studies. Implications: Ozone source attribution results provide useful information on important emission source contribution categories and provide some initial guidance on future emission reduction strategies. This study explains a new source apportionment technique, CMAQ-ISAM, and compares it to CAMx OSAT. The techniques have similar results: ozone's highest source contributor is boundary conditions, followed by point sources, then off-road mobile sources. The current version of ISAM in CMAQ 5.0.2 requires significant computing resources for ozone source attribution, while the computing requirements for PM source attribution are even more onerous. CMAQ 5.2 was released after this study was completed, and does not include ISAM.

Future-year ozone prediction for the United States using updated models and inputs.

The relationship between emission reductions and changes in ozone can be studied using photochemical grid models. These models are updated with new information as it becomes available. The primary objective of this study was to update the previous Collet et al. studies by using the most up-to-date (at the time the study was done) modeling emission tools, inventories, and meteorology available to conduct ozone source attribution and sensitivity studies. Results show future-year, 2030, design values for 8-hr ozone concentrations were lower than base-year values, 2011. The ozone source attribution results for selected cities showed that boundary conditions were the dominant contributors to ozone concentrations at the western U.S. locations, and were important for many of the eastern U.S. LOCATIONS: Point sources were generally more important in the eastern United States than in the western United States. The contributions of on-road mobile emissions were less than 5 ppb at a majority of the cities selected for analysis. The higher-order decoupled direct method (HDDM) results showed that in most of the locations selected for analysis, NOx emission reductions were more effective than VOC emission reductions in reducing ozone levels. The source attribution results from this study provide useful information on the important source categories and provide some initial guidance on future emission reduction strategies. IMPLICATIONS: The relationship between emission reductions and changes in ozone can be studied using photochemical grid models, which are updated with new available information. This study was to update the previous Collet et al. studies by using the most current, at the time the study was done, models and inventory to conduct ozone source attribution and sensitivity studies. The source attribution results from this study provide useful information on the important source categories and provide some initial guidance on future emission reduction strategies.

Implementation and application of sub-grid-scale plume treatment in the latest version of EPA's third-generation air quality model, CMAQ 5.01.

UNLABELLED: The Community Multiscale Air Quality (CMAQ) modeling system Version 5.0 (CMAQv5.0) was released by the US. Environmental Protection Agency (EPA) in February 2012, with an interim release (v5.01) in July 2012. Because CMAQ is a community model, the EPA encourages the development of proven alternative science treatments by external scientists and developers that can be incorporated as part of an official CMAQ release. This paper describes the implementation, evaluation, and testing of a plume-in-grid (PinG) module in CMAQ 5.01. The PinG module, also referred to as Advanced Plume Treatment (APT), provides the capability of resolving sub-grid-scale processes, such as the transport and chemistry of point-source plumes, in a grid model. The new PinG module in CMAQ 5.01 is applied and evaluated for two 15-day summer and winter periods in 2005 to the eastern United States, and the results are compared with those from the base CMAQ 5.01. Eighteen large point sources of NO(x) in the eastern United States were selected for explicit plume treatment with APT in the PinG simulation. The results show that overall model performance is negligibly affected when PinG treatment is included. However the PinG model predicts significantly different contributions of the 18 sources to pollutant concentrations and deposition downwind of the point sources compared to the base model. IMPLICATIONS: This study describes the incorporation of a plume-in-grid (PinG) capability within the latest version of the EPA grid model, CMAQ. The capability addresses the inherent limitation of the grid model to resolve processes, such as the evolution of point-source plumes, which occur at scales much smaller than the grid resolution. The base grid model and the PinG version predict different source contributions to ozone and PM2.5 concentrations that need to be considered when source attribution studies are conducted to determine the impacts of large point sources on downwind concentrations and deposition of primary and secondary pollutants.

Evaluation of light-duty vehicle mobile source regulations on ozone concentration trends in 2018 and 2030 in the western and eastern United States.

To improve U.S. air quality, there are many regulations on-the-way (OTW) and on-the-books (OTB), including mobile source California Low Emission Vehicle third generation (LEV III) and federal Tier 3 standards. This study explores the effects of those regulations by using the U.S. Environmental Protection Agency's (EPA) Community Multiscale Air Quality (CMAQ) model for 8-hr ozone concentrations in the western and eastern United States in the years 2018 and 2030 during a month with typical high ozone concentrations, July. Alterations in pollutant emissions can be due to technological improvements, regulatory amendments, and changes in growth. In order to project emission rates for future years, the impacts of all of these factors were estimated. This study emphasizes the potential light-duty vehicle emission changes by year to predict ozone levels. The results of this study show that most areas have decreases in 8-hr ozone concentrations in the year 2030, although there are some areas with increased concentrations. Additionally, there are areas with 8-hr ozone concentrations greater than the current US. National Ambient Air Quality Standard level, which is 75 ppb.

A case study of the relative effects of power plant nitrogen oxides and sulfur dioxide emission reductions on atmospheric nitrogen deposition.

The contrasting effects of point source nitrogen oxides (NOx) and sulfur dioxide (SO2) air emission reductions on regional atmospheric nitrogen deposition are analyzed for the case study of a coal-fired power plant in the southeastern United States. The effect of potential emission reductions at the plant on nitrogen deposition to Escambia Bay and its watershed on the Florida-Alabama border is simulated using the three-dimensional Eulerian Community Multiscale Air Quality (CMAQ) model. A method to quantify the relative and individual effects of NOx versus SO2 controls on nitrogen deposition using air quality modeling results obtained from the simultaneous application of NOx and SO2 emission controls is presented and discussed using the results from CMAQ simulations conducted with NOx-only and SO2-only emission reductions; the method applies only to cases in which ambient inorganic nitrate is present mostly in the gas phase; that is, in the form of gaseous nitric acid (HNO3). In such instances, the individual effects of NOx and SO2 controls on nitrogen deposition can be approximated by the effects of combined NOx + SO2 controls on the deposition of NOy, (the sum of oxidized nitrogen species) and reduced nitrogen species (NHx), respectively. The benefit of controls at the plant in terms of the decrease in nitrogen deposition to Escambia Bay and watershed is less than 6% of the overall benefit due to regional Clean Air Interstate Rule (CAIR) controls.

Global source attribution for mercury deposition in the United States.

A multiscale modeling system that consists of a global chemical transport model (CTM) and a nested continental CTM was used to simulate the global atmospheric fate and transport of mercury and its deposition over the contiguous United States. The performance of the CTMs was evaluated against available data. The coefficient of determination (r2) for observed versus simulated annual mercury wet deposition fluxes over North America was 0.50 with average normalized error and bias of 25% and 11%, respectively. The CTMs were used to conduct a global source attribution for selected receptor areas. Three global emission scenarios were used that differed in their distribution of background emissions among direct natural emissions and re-emissions of natural and anthropogenic mercury. North American anthropogenic sources were calculated to contribute only from 25 to 32% to the total mercury deposition over the continental United States. At selected receptors, the contribution of North American anthropogenic emissions ranges from 9 to 81%; Asian anthropogenic emissions were calculated to contribute from 5 to 36%; natural emissions were calculated to contribute from 6 to 59%.

On the effect of spatial resolution on atmospheric mercury modeling.

Mathematical modeling of the atmospheric fate and transport of mercury (Hg) was conducted using three nested domains covering global, continental and regional scales with horizontal resolutions of approximately 1000, 100 and 20 km, respectively. Comparisons of modeling results with wet deposition fluxes show a coefficient of determination (r(2)) of 0.45 for the continental simulation and 0.14 for the continental/regional simulation. The poor correlation obtained in the regional simulation results to a large extent from the fact that the model predicts an increasing gradient in Hg wet deposition from Minnesota to Pennsylvania, which is not observed in the monitoring network. The use of a finer spatial resolution (20 km) improves model performance in Minnesota and Wisconsin (upwind of major Hg emission sources) but degrades model performance in Pennsylvania (downwind of major Hg emission sources). We suggest the hypothesis that some key Hg chemical transformations are likely missing in current models of atmospheric Hg.

Simulation of Sulfate and Nitrate Chemistry in Power Plant Plumes.

The rate of formation of secondary particulate matter (PM) in power plant plumes varies as the plume material mixes with the background air. Consequently, the rate of oxidation of sulfur dioxide (SO2) and nitrogen dioxide (NO2) to sulfate and nitric acid, respectively, can be very different in plumes and in the background air (i.e., air outside the plume). In addition, the formation of sulfate and nitric acid in a power plant plume is a strong function of the chemical composition of the background air and the prevailing meteorological conditions. We describe the use of a reactive plume model, the Reactive and Optics Model of Emissions, to simulate sulfate and nitrate formation in a power plant plume for a variety of background conditions. We show that SO2 and NO2 oxidation rates are maximum in the background air for volatile organic compound (VOC)-limited airsheds but are maximum at some downwind distance in the plume when the background air is nitrogen oxide (NOx)-limited. Our analysis also shows that it is essential to obtain measurements of background concentrations of ozone, aldehydes, peroxyacetyl nitrate, and other VOCs to properly describe plume chemistry.

The Development of a Model to Examine Source-Receptor Relationships for Visibility on the Colorado Plateau.

This paper describes the development and application of the Visibility and Haze in the Western Atmosphere (VISHWA) model to understand the source-receptor relationships that govern chemical species relevant to visibility degradation in the western United States. The model was developed as part of a project referred to as Visibility Assessment for Regional Emission Distributions (VARED), the objective of which is to estimate the contributions of various geographical regions, compounds, and emission sources to light scattering and absorption by particles on the Colorado Plateau. The VISHWA model is a modified version of a comprehensive Eulerian model, known as the Acid Deposition and Oxidant Model.1 The modifications were designed to obtain the computational efficiency required to simulate a one-year period at about 1/25th of real time, and at the same time incorporate mechanistic features relevant to realistic modeling of the fate and transport of visibility degrading species. The modifications included use of a condensed chemical mechanism; incorporation of reactions to simulate the formation of secondary organic particles; and use of a semi-Lagrangian advection scheme to preserve concentration peaks during advection. The model was evaluated with 1992 air quality data from Project MOHAVE (Measurements of Haze and Visual Effects) intensive experiments. An important conclusion of this evaluation is that aqueous-phase oxidation of SO2 to sulfate in nonprecipitating clouds makes a significant contribution to observed sulfate levels during winter as well as summer. Model estimates of ambient sulfate for the winter intensive were within a factor of 2 of the observations for 75% of the values. The corresponding statistic for the summer intensive was 90%. Model estimates of carbon were within a factor of 2 of the limited set of observations.