Evaluation of 15 years of modeled atmospheric oxidized nitrogen compounds across the contiguous United States.

Atmospheric nitrogen oxide and nitrogen dioxide (NO + NO2, together termed as NO X ) estimates from annual photochemical simulations for years 2002-2016 are compared to surface network measurements of NO X and total gas-phase-oxidized reactive nitrogen (NO Y ) to evaluate the Community Multiscale Air Quality (CMAQ) modeling system performance by U.S. region, season, and time of day. In addition, aircraft measurements from 2011 Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality are used to evaluate how emissions, chemical mechanism, and measurement uncertainty each contribute to the overall model performance. We show distinct seasonal and time-of-day patterns in NO X performance. Summertime NO X is overpredicted with bimodal peaks in bias during early morning and evening hours and persisting overnight. The summertime morning NO X bias dropped from between 28% and 57% for earlier years (2002-2012) to between -2% and 7% for later years (2013-2016). Summer daytime NO X tends to be unbiased or underpredicted. In winter, the evening NO X overpredictions remain, but NO X is unbiased or underpredicted overnight, in the morning, and during the day. NO X overpredictions are most pronounced in the Midwestern and Southern United States with Western regions having more of a tendency toward model underpredictions of NO X . Modeled NO X performance has improved substantially over time, reflecting updates to the emission inputs and the CMAQ air quality model. Model performance improvements are largest for years simulated with CMAQv5.1 or later and for emission inventory years 2014 and later, coinciding with reduced onroad NO X emissions from vehicles with newer emission control technologies and improved treatment of chemistry, deposition, and vertical mixing in CMAQ. Our findings suggest that emissions temporalization of specific mobile source sectors have a small impact on model performance, while chemistry updates improve predictions of NO Y but do not improve summertime NO X bias in the Baltimore/DC area. Sensitivity runs performed for different locations across the country suggest that the improvement in summer NO X performance can be attributed to updates in vertical mixing incorporated in CMAQv5.1.

Examining PM2.5 concentrations and exposure using multiple models.

Epidemiologic studies have found associations between fine particulate matter (PM2.5) exposure and adverse health effects using exposure models that incorporate monitoring data and other relevant information. Here, we use nine PM2.5 concentration models (i.e., exposure models) that span a wide range of methods to investigate i) PM2.5 concentrations in 2011, ii) potential changes in PM2.5 concentrations between 2011 and 2028 due to on-the-books regulations, and iii) PM2.5 exposure for the U.S. population and four racial/ethnic groups. The exposure models included two geophysical chemical transport models (CTMs), two interpolation methods, a satellite-derived aerosol optical depth-based method, a Bayesian statistical regression model, and three data-rich machine learning methods. We focused on annual predictions that were regridded to 12-km resolution over the conterminous U.S., but also considered 1-km predictions in sensitivity analyses. The exposure models predicted broadly consistent PM2.5 concentrations, with relatively high concentrations on average over the eastern U.S. and greater variability in the western U.S. However, differences in national concentration distributions (median standard deviation: 1.00 µg m-3) and spatial distributions over urban areas were evident. Further exploration of these differences and their implications for specific applications would be valuable. PM2.5 concentrations were estimated to decrease by about 1 µg m-3 on average due to modeled emission changes between 2011 and 2028, with decreases of more than 3 µg m-3 in areas with relatively high 2011 concentrations that were projected to experience relatively large emission reductions. Agreement among models was closer for population-weighted than uniformly weighted averages across the domain. About 50% of the population was estimated to experience PM2.5 concentrations less than 10 µg m-3 in 2011 and PM2.5 improvements of about 2 µg m-3 due to modeled emission changes between 2011 and 2028. Two inequality metrics were used to characterize differences in exposure among the four racial/ethnic groups. The metrics generally yielded consistent information and suggest that the modeled emission reductions between 2011 and 2028 would reduce absolute exposure inequality on average.

Assessing PM2.5 Model Performance for the Conterminous U.S. with Comparison to Model Performance Statistics from 2007-2015.

Previous studies have proposed that model performance statistics from earlier photochemical grid model (PGM) applications can be used to benchmark performance in new PGM applications. A challenge in implementing this approach is that limited information is available on consistently calculated model performance statistics that vary spatially and temporally over the U.S. Here, a consistent set of model performance statistics are calculated by year, season, region, and monitoring network for PM2.5 and its major components using simulations from versions 4.7.1-5.2.1 of the Community Multiscale Air Quality (CMAQ) model for years 2007-2015. The multi-year set of statistics is then used to provide quantitative context for model performance results from the 2015 simulation. Model performance for PM2.5 organic carbon in the 2015 simulation ranked high (i.e., favorable performance) in the multi-year dataset, due to factors including recent improvements in biogenic secondary organic aerosol and atmospheric mixing parameterizations in CMAQ. Model performance statistics for the Northwest region in 2015 ranked low (i.e., unfavorable performance) for many species in comparison to the 2007-2015 dataset. This finding motivated additional investigation that suggests a need for improved speciation of wildfire PM2.5emissions and modeling of boundary layer dynamics near water bodies. Several limitations were identified in the approach of benchmarking new model performance results with previous results. Since performance statistics vary widely by region and season, a simple set of national performance benchmarks (e.g., one or two targets per species and statistic) as proposed previously are inadequate to assess model performance throughout the U.S. Also, trends in model performance statistics for sulfate over the 2007 to 2015 period suggest that model performance for earlier years may not be a useful reference for assessing model performance for recent years in some cases. Comparisons of results from the 2015 base case with results from five sensitivity simulations demonstrated the importance of parameterizations of NH3 surface exchange, organic aerosol volatility and production, and emissions of crustal cations for predicting PM2.5 species concentrations.

A System for Developing and Projecting PM2.5 Spatial Fields to Correspond to Just Meeting National Ambient Air Quality Standards.

PM2.5 concentration fields that correspond to just meeting national ambient air quality standards (NAAQS) are useful for characterizing exposure in regulatory assessments. Computationally efficient methods that incorporate predictions from photochemical grid models (PGM) are needed to realistically project baseline concentration fields for these assessments. Thorough cross validation (CV) of hybrid spatial prediction models is also needed to better assess their predictive capability in sparsely monitored areas. In this study, a system for generating, evaluating, and projecting PM2.5 spatial fields to correspond with just meeting the PM2.5 NAAQS is developed and demonstrated. Results of ten-fold CV based on standard and spatial cluster withholding approaches indicate that performance of three spatial prediction models improves with decreasing distance to the nearest neighboring monitor, improved PGM performance, and increasing distance from sources of PM2.5 heterogeneity (e.g., complex terrain and fire). An air quality projection tool developed here is demonstrated to be effective for quickly projecting PM2.5 spatial fields to just meet NAAQS using realistic spatial response patterns based on air quality modeling. PM2.5 tends to be most responsive to primary PM2.5 emissions in urban areas, whereas response patterns are relatively smooth for NOx and SO2 emission changes. On average, PM2.5 is more responsive to changes in anthropogenic primary PM2.5 emissions than NOx and SO2 emissions in the contiguous U.S.

The estimated change in the level and distribution of PM2.5-attributable health impacts in the United States: 2005-2014.

BACKGROUND: Photochemical modeling can predict the level and distribution of pollutant concentrations over time, but is resource-intensive. Partly for this reason, there are few studies exploring the multi-year trajectory of the historical change in fine particle (PM2.5) levels and associated health impacts in the U.S. OBJECTIVES: We used a unique dataset of Community Multi-Scale Air Quality (CMAQ) model simulations performed for a subset of years over a decade-long period fused with observations to estimate the change in ambient levels of PM2.5 across the contiguous U.S. We also quantified the change in PM2.5-attributable health risks and characterized the level of risk inequality over this period. METHODS: We estimated annual mean PM2.5 concentrations in 2005, 2011 and 2014. Using log-linear and logistic concentration-response coefficients we estimated changes in the numbers of deaths, hospital admissions and other morbidity outcomes. Calculating the Gini coefficient and Atkinson Index, we characterized the extent to which PM2.5 attributable risks were shared equally across the population or instead concentrated among certain subgroups. RESULTS: In 2005 the estimated fraction of deaths due to PM2.5 was 6.1%. This estimated value falls to 4.6% by 2014. Every portion of the contiguous U.S. experiences a decline in the risk of PM-related premature death over the 10-year period. As measured by the Gini coefficient and Atkinson index, the level of PM mortality risk is shared more equally in 2014 than in 2005 among all subgroups. CONCLUSIONS: Between 2005 and 2014, the level of PM2.5 concentrations fall, and the risk of premature death, declined and became more equitably distributed across the U.S.

Recommended metric for tracking visibility progress in the Regional Haze Rule.

For many national parks and wilderness areas with special air quality protections (Class I areas) in the western United States (U.S.), wildfire smoke and dust events can have a large impact on visibility. The U.S. Environmental Protection Agency's (EPA) 1999 Regional Haze Rule used the 20% haziest days to track visibility changes over time even if they are dominated by smoke or dust. Visibility on the 20% haziest days has remained constant or degraded over the last 16 yr at some Class I areas despite widespread emission reductions from anthropogenic sources. To better track visibility changes specifically associated with anthropogenic pollution sources rather than natural sources, the EPA has revised the Regional Haze Rule to track visibility on the 20% most anthropogenically impaired (hereafter, most impaired) days rather than the haziest days. To support the implementation of this revised requirement, the EPA has proposed (but not finalized) a recommended metric for characterizing the anthropogenic and natural portions of the daily extinction budget at each site. This metric selects the 20% most impaired days based on these portions using a "delta deciview" approach to quantify the deciview scale impact of anthropogenic light extinction. Using this metric, sulfate and nitrate make up the majority of the anthropogenic extinction in 2015 on these days, with natural extinction largely made up of organic carbon mass in the eastern U.S. and a combination of organic carbon mass, dust components, and sea salt in the western U.S. For sites in the western U.S., the seasonality of days selected as the 20% most impaired is different than the seasonality of the 20% haziest days, with many more winter and spring days selected. Applying this new metric to the 2000-2015 period across sites representing Class I areas results in substantial changes in the calculated visibility trend for the northern Rockies and southwest U.S., but little change for the eastern U.S. IMPLICATIONS: Changing the approach for tracking visibility in the Regional Haze Rule allows the EPA, states, and the public to track visibility on days when reductions in anthropogenic emissions have the greatest potential to improve the view. The calculations involved with the recommended metric can be incorporated into the routine IMPROVE (Interagency Monitoring of Protected Visual Environments) data processing, enabling rapid analysis of current and future visibility trends. Natural visibility conditions are important in the calculations for the recommended metric, necessitating the need for additional analysis and potential refinement of their values.

Characterizing CO and NO y Sources and Relative Ambient Ratios in the Baltimore Area Using Ambient Measurements and Source Attribution Modeling.

Modeled source attribution information from the Community Multiscale Air Quality model was coupled with ambient data from the 2011 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality Baltimore field study. We assess source contributions and evaluate the utility of using aircraft measured CO and NO y relationships to constrain emission inventories. We derive ambient and modeled ΔCO:ΔNO y ratios that have previously been interpreted to represent CO:NO y ratios in emissions from local sources. Modeled and measured ΔCO:ΔNO y are similar; however, measured ΔCO:ΔNO y has much more daily variability than modeled values. Sector-based tagging shows that regional transport, on-road gasoline vehicles, and nonroad equipment are the major contributors to modeled CO mixing ratios in the Baltimore area. In addition to those sources, on-road diesel vehicles, soil emissions, and power plants also contribute substantially to modeled NO y in the area. The sector mix is important because emitted CO:NO x ratios vary by several orders of magnitude among the emission sources. The model-predicted gasoline/diesel split remains constant across all measurement locations in this study. Comparison of ΔCO:ΔNO y to emitted CO:NO y is challenged by ambient and modeled evidence that free tropospheric entrainment, and atmospheric processing elevates ambient ΔCO:ΔNO y above emitted ratios. Specifically, modeled ΔCO:ΔNO y from tagged mobile source emissions is enhanced 5-50% above the emitted ratios at times and locations of aircraft measurements. We also find a correlation between ambient formaldehyde concentrations and measured ΔCO:ΔNO y suggesting that secondary CO formation plays a role in these elevated ratios. This analysis suggests that ambient urban daytime ΔCO:ΔNO y values are not reflective of emitted ratios from individual sources.

A direct sensitivity approach to predict hourly ozone resulting from compliance with the National Ambient Air Quality Standard.

In setting primary ambient air quality standards, the EPA's responsibility under the law is to establish standards that protect public health. As part of the current review of the ozone National Ambient Air Quality Standard (NAAQS), the US EPA evaluated the health exposure and risks associated with ambient ozone pollution using a statistical approach to adjust recent air quality to simulate just meeting the current standard level, without specifying emission control strategies. One drawback of this purely statistical concentration rollback approach is that it does not take into account spatial and temporal heterogeneity of ozone response to emissions changes. The application of the higher-order decoupled direct method (HDDM) in the community multiscale air quality (CMAQ) model is discussed here to provide an example of a methodology that could incorporate this variability into the risk assessment analyses. Because this approach includes a full representation of the chemical production and physical transport of ozone in the atmosphere, it does not require assumed background concentrations, which have been applied to constrain estimates from past statistical techniques. The CMAQ-HDDM adjustment approach is extended to measured ozone concentrations by determining typical sensitivities at each monitor location and hour of the day based on a linear relationship between first-order sensitivities and hourly ozone values. This approach is demonstrated by modeling ozone responses for monitor locations in Detroit and Charlotte to domain-wide reductions in anthropogenic NOx and VOCs emissions. As seen in previous studies, ozone response calculated using HDDM compared well to brute-force emissions changes up to approximately a 50% reduction in emissions. A new stepwise approach is developed here to apply this method to emissions reductions beyond 50% allowing for the simulation of more stringent reductions in ozone concentrations. Compared to previous rollback methods, this application of modeled sensitivities to ambient ozone concentrations provides a more realistic spatial response of ozone concentrations at monitors inside and outside the urban core and at hours of both high and low ozone concentrations.