A hybrid approach to predict daily NO2 concentrations at city block scale.

Estimating the ambient concentration of nitrogen dioxide (NO2) is challenging because NO2 generated by local fossil fuel combustion varies greatly in concentration across space and time. This study demonstrates an integrated hybrid approach combining dispersion modeling and land use regression (LUR) to predict daily NO2 concentrations at a high spatial resolution (e.g., 50 m) in the New York tri-state area. The daily concentration of traffic-related NO2 was estimated at the Environmental Protection Agency's NO2 monitoring sites in the study area for the years 2015-2017, using the Research LINE source (R-LINE) model with inputs of traffic data provided by the Highway Performance and Management System and meteorological data provided by the NOAA Integrated Surface Database. We used the R-LINE-predicted daily concentrations of NO2 to build mixed-effects regression models, including additional variables representing land use features, geographic characteristics, weather, and other predictors. The mixed model was selected by the Elastic Net method. Each model's performance was evaluated using the out-of-sample coefficient of determination (R2) and the square root of mean squared error (RMSE) from ten-fold cross-validation (CV). The mixed model showed a good prediction performance (CV R2: 0.75-0.79, RMSE: 3.9-4.0 ppb). R-LINE outputs improved the overall, spatial, and temporal CV R2 by 10.0%, 18.9% and 7.7% respectively. Given the output of R-LINE is point-based and has a flexible spatial resolution, this hybrid approach allows prediction of daily NO2 at an extremely high spatial resolution such as city blocks.

Assessing Model Characterization of Single Source Secondary Pollutant Impacts Using 2013 SENEX Field Study Measurements.

Aircraft measurements made downwind from specific coal fired power plants during the 2013 Southeast Nexus field campaign provide a unique opportunity to evaluate single source photochemical model predictions of both O3 and secondary PM2.5 species. The model did well at predicting downwind plume placement. The model shows similar patterns of an increasing fraction of PM2.5 sulfate ion to the sum of SO2 and PM2.5 sulfate ion by distance from the source compared with ambient based estimates. The model was less consistent in capturing downwind ambient based trends in conversion of NOX to NOY from these sources. Source sensitivity approaches capture near-source O3 titration by fresh NO emissions, in particular subgrid plume treatment. However, capturing this near-source chemical feature did not translate into better downwind peak estimates of single source O3 impacts. The model estimated O3 production from these sources but often was lower than ambient based source production. The downwind transect ambient measurements, in particular secondary PM2.5 and O3, have some level of contribution from other sources which makes direct comparison with model source contribution challenging. Model source attribution results suggest contribution to secondary pollutants from multiple sources even where primary pollutants indicate the presence of a single source.

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning.

Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustion sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds-water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May-June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from -5.62 to -2.42 µg m-3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73µg m-3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes.

Chemical transport model simulations of organic aerosol in southern California: model evaluation and gasoline and diesel source contributions.

Gasoline- and diesel-fueled engines are ubiquitous sources of air pollution in urban environments. They emit both primary particulate matter and precursor gases that react to form secondary particulate matter in the atmosphere. In this work, we updated the organic aerosol module and organic emissions inventory of a three-dimensional chemical transport model, the Community Multiscale Air Quality Model (CMAQ), using recent, experimentally derived inputs and parameterizations for mobile sources. The updated model included a revised volatile organic compound (VOC) speciation for mobile sources and secondary organic aerosol (SOA) formation from unspeciated intermediate volatility organic compounds (IVOCs). The updated model was used to simulate air quality in southern California during May and June 2010, when the California Research at the Nexus of Air Quality and Climate Change (CalNex) study was conducted. Compared to the Traditional version of CMAQ, which is commonly used for regulatory applications, the updated model did not significantly alter the predicted organic aerosol (OA) mass concentrations but did substantially improve predictions of OA sources and composition (e.g., POA-SOA split), as well as ambient IVOC concentrations. The updated model, despite substantial differences in emissions and chemistry, performed similar to a recently released research version of CMAQ (Woody et al., 2016) that did not include the updated VOC and IVOC emissions and SOA data. Mobile sources were predicted to contribute 30-40 % of the OA in southern California (half of which was SOA), making mobile sources the single largest source contributor to OA in southern California. The remainder of the OA was attributed to non-mobile anthropogenic sources (e.g., cooking, biomass burning) with biogenic sources contributing to less than 5 % to the total OA. Gasoline sources were predicted to contribute about 13 times more OA than diesel sources; this difference was driven by differences in SOA production. Model predictions highlighted the need to better constrain multi-generational oxidation reactions in chemical transport models.

Estimating State-Specific Contributions to PM2.5- and O3-Related Health Burden from Residential Combustion and Electricity Generating Unit Emissions in the United States.

BACKGROUND: Residential combustion (RC) and electricity generating unit (EGU) emissions adversely impact air quality and human health by increasing ambient concentrations of fine particulate matter (PM2.5) and ozone (O3). Studies to date have not isolated contributing emissions by state of origin (source-state), which is necessary for policy makers to determine efficient strategies to decrease health impacts. OBJECTIVES: In this study, we aimed to estimate health impacts (premature mortalities) attributable to PM2.5 and O3 from RC and EGU emissions by precursor species, source sector, and source-state in the continental United States for 2005. METHODS: We used the Community Multiscale Air Quality model employing the decoupled direct method to quantify changes in air quality and epidemiological evidence to determine concentration-response functions to calculate associated health impacts. RESULTS: We estimated 21,000 premature mortalities per year from EGU emissions, driven by sulfur dioxide emissions forming PM2.5. More than half of EGU health impacts are attributable to emissions from eight states with significant coal combustion and large downwind populations. We estimate 10,000 premature mortalities per year from RC emissions, driven by primary PM2.5 emissions. States with large populations and significant residential wood combustion dominate RC health impacts. Annual mortality risk per thousand tons of precursor emissions (health damage functions) varied significantly across source-states for both source sectors and all precursor pollutants. CONCLUSIONS: Our findings reinforce the importance of pollutant-specific, location-specific, and source-specific models of health impacts in design of health-risk minimizing emissions control policies. Citation: Penn SL, Arunachalam S, Woody M, Heiger-Bernays W, Tripodis Y, Levy JI. 2017. Estimating state-specific contributions to PM2.5- and O3-related health burden from residential combustion and electricity generating unit emissions in the United States. Environ Health Perspect 125:324-332; http://dx.doi.org/10.1289/EHP550.

Current and future particulate-matter-related mortality risks in the United States from aviation emissions during landing and takeoff.

Demand for air travel is projected to increase in the upcoming years, with a corresponding influence on emissions, air quality, and public health. The trajectory of health impacts would be influenced by not just emissions growth, but also changes in nonaviation ambient concentrations that influence secondary fine particulate matter (PM(2.5) ) formation, population growth and aging, and potential shifts in PM(2.5) concentration-response functions (CRFs). However, studies to date have not systematically evaluated the individual and joint contributions of these factors to health risk trajectories. In this study, we simulated emissions during landing and takeoff from aircraft at 99 airports across the United States for 2005 and for a 2025 flight activity projection scenario. We applied the Community Multiscale Air Quality (CMAQ) model with the Speciated Modeled Attainment Test (SMAT) to determine the contributions of these emissions to ambient concentrations, including scenarios with 2025 aircraft emissions and 2005 nonaviation air quality. We combined CMAQ outputs with PM(2.5) mortality CRFs and population projections, and evaluated the influence of changing emissions, nonaviation concentrations, and population factors. Given these scenarios, aviation-related health impacts would increase by a factor of 6.1 from 2005 to 2025, with a factor of 2.1 attributable to emissions, a factor of 1.3 attributable to population factors, and a factor of 2.3 attributable to changing nonaviation concentrations which enhance secondary PM(2.5) formation. Our study emphasizes that the public health burden of aviation emissions would be significantly influenced by the joint effects of flight activity increases, nonaviation concentration changes, and population growth and aging.