2002-2017 anthropogenic emissions data for air quality modeling over the United States.

The United States Environmental Protection Agency (US EPA) has developed a set of annual North American emissions data for multiple air pollutants across 18 broad source categories for 2002 through 2017. The sixteen new annual emissions inventories were developed using consistent input data and methods across all years. When a consistent method or tool was not available for a source category, emissions were estimated by scaling data from the EPA's 2017 National Emissions Inventory with scaling factors based on activity data and/or emissions control information. The emissions datasets are designed to support regional air quality modeling for a wide variety of human health and ecological applications. The data were developed to support simulations of the EPA's Community Multiscale Air Quality model but can also be used by other regional scale air quality models. The emissions data are one component of EPA's Air Quality Time Series Project which also includes air quality modeling inputs (meteorology, initial conditions, boundary conditions) and outputs (e.g., ozone, PM2.5 and constituent species, wet and dry deposition) for the Conterminous US at a 12 km horizontal grid spacing.

The Community Multiscale Air Quality (CMAQ) model versions 5.3 and 5.3.1: system updates and evaluation.

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by version 5.3.1 (CMAQ531) in December 2019, contains numerous science updates, enhanced functionality, and improved computation efficiency relative to the previous version of the model, 5.2.1 (CMAQ521). Major science advances in the new model include a new aerosol module (AERO7) with significant updates to secondary organic aerosol (SOA) chemistry, updated chlorine chemistry, updated detailed bromine and iodine chemistry, updated simple halogen chemistry, the addition of dimethyl sulfide (DMS) chemistry in the CB6r3 chemical mechanism, updated M3Dry bidirectional deposition model, and the new Surface Tiled Aerosol and Gaseous Exchange (STAGE) bidirectional deposition model. In addition, support for the Weather Research and Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added to CMAQ53 and the Meteorology-Chemistry Interface Processor (MCIP) version 5.0 (MCIP50). Enhanced functionality in CMAQ53 includes the new Detailed Emissions Scaling, Isolation and Diagnostic (DESID) system for scaling incoming emissions to CMAQ and reading multiple gridded input emission files. Evaluation of CMAQ531 was performed by comparing monthly and seasonal mean daily 8 h average (MDA8) O3 and daily PM2.5 values from several CMAQ531 simulations to a similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O3, CMAQ531 has higher O3 in the winter versus CMAQ521, due primarily to reduced dry deposition to snow, which strongly reduces wintertime O3 bias (2-4 ppbv monthly average). MDA8 O3 is lower with CMAQ531 throughout the rest of the year, particularly in spring, due in part to reduced O3 from the lateral boundary conditions (BCs), which generally increases MDA8 O3 bias in spring and fall ( 0.5 µg m-3). For daily 24 h average PM2.5, CMAQ531 has lower concentrations on average in spring and fall, higher concentrations in summer, and similar concentrations in winter to CMAQ521, which slightly increases bias in spring and fall and reduces bias in summer. Comparisons were also performed to isolate updates to several specific aspects of the modeling system, namely the lateral BCs, meteorology model version, and the deposition model used. Transitioning from a hemispheric CMAQ (HCMAQ) version 5.2.1 simulation to a HCMAQ version 5.3 simulation to provide lateral BCs contributes to higher O3 mixing ratios in the regional CMAQ simulation in higher latitudes during winter (due to the decreased O3 dry deposition to snow in CMAQ53) and lower O3 mixing ratios in middle and lower latitudes year-round (due to reduced O3 over the ocean with CMAQ53). Transitioning from WRF version 3.8 to WRF version 4.1.1 with the HVC resulted in consistently higher (1.0-1.5 ppbv) MDA8 O3 mixing ratios and higher PM2.5 concentrations (0.1-0.25 µg m-3) throughout the year. Finally, comparisons of the M3Dry and STAGE deposition models showed that MDA8 O3 is generally higher with M3Dry outside of summer, while PM2.5 is consistently higher with STAGE due to differences in the assumptions of particle deposition velocities to non-vegetated surfaces and land use with short vegetation (e.g., grasslands) between the two models. For ambient NH3, STAGE has slightly higher concentrations and smaller bias in the winter, spring, and fall, while M3Dry has higher concentrations and smaller bias but larger error and lower correlation in the summer.

Significant ground-level ozone attributed to lightning-induced nitrogen oxides during summertime over the Mountain West States.

Using lightning flash data from the National Lightning Detection Network with an updated lightning nitrogen oxides (NOx) emission estimation algorithm in the Community Multiscale Air Quality (CMAQ) model, we estimate the hourly variations in lightning NOx emissions for the summer of 2011 and simulate its impact on distributions of tropospheric ozone (O3) across the continental United States. We find that typical summer-time lightning activity across the U.S. Mountain West States (MWS) injects NOx emissions comparable to those from anthropogenic sources into the troposphere over the region. Comparison of two model simulation cases with and without lightning NOx emissions show that significant amount of ground-level O3 in the MWS during the summer can be attributed to the lightning NOX emissions. The simulated surface-level O3 from a model configuration incorporating lightning NOx emissions showed better agreement with the observed values than the model configuration without lightning NOx emissions. The time periods of significant reduction in bias in simulated O3 between these two cases strongly correlate with the time periods when lightning activity occurred in the region. The inclusion of lightning NOx increased daily maximum 8 h O3 by up to 17 ppb and improved model performance relative to measured surface O3 mixing ratios in the MWS region. Analysis of model results in conjunction with lidar measurements at Boulder, Colorado during July 2014 corroborated similar impacts of lightning NOx emissions on O3 emissions estimated for other summers is comparable to the 2011 air quality. The magnitude of lightning NOx estimates suggesting that summertime surface-level O3 levels in the MWS region could be significantly influenced by lightning NOx.

Influence of uncertainties in burned area estimates on modeled wildland fire PM2.5 and ozone pollution in the contiguous U.S.

Wildland fires are a major source of fine particulate matter (PM2.5), one of the most harmful ambient pollutants for human health globally. To represent the influence of wildland fire emissions on atmospheric composition, regional and global chemical transport models rely on emission inventories developed from estimates of burned area (i.e. fire size and location). While different methods of estimating annual burned area agree reasonably well in the western U.S. (within 20-30% for most years during 2002-2014), estimates for the southern U.S. can vary by more than a factor of 5. These differences in burned area lead to significant variability in the spatial and temporal allocation of emissions across fire emission inventory platforms. In this work, we implement wildland fire emission estimates for 2011 from three different products - the USEPA National Emission Inventory (NEI), the Fire Inventory of NCAR (FINN), and the Global Fire Emission Database (GFED4s) - into the Community Multiscale Air Quality (CMAQ) model to quantify and characterize differences in simulated PM and ozone concentrations across the contiguous U.S. (CONUS) due to the fire emission inventory used. The NEI is developed specifically for the U.S., while both FINN and GFED4s are available globally. We find that NEI emissions lead to the largest increases in modeled annual average PM2.5 (0.85 µg m-3) and April-September maximum daily 8-h ozone (0.28 ppb) nationally compared to a "no fire" baseline, followed by FINN (0.33 µg m-3 and 0.22 ppb) and GFED4s (0.12 µg m-3 and 0.17 ppb). Annual mean enhancements in wildland fire pollution are highest in the southern U.S. across all three inventories (over 4 µg m-3 and 2 ppb in some areas), but show considerable spatial variability within these regions. We also examine the representation of five individual fire events during 2011 and find that of the two global inventories, FINN reproduces more of the acute changes in pollutant concentrations modeled with NEI and shown in surface observations during each of the episodes investigated compared to GFED4s. Understanding the sensitivity of modeling fire-related PM2.5 and ozone in the U.S. to burned area estimation approaches will inform future efforts to assess the implications of present and future fire activity for air quality and human health at national and global scales.

Description and evaluation of the Community Multiscale Air Quality (CMAQ) modeling system version 5.1.

The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system developed and maintained by the US Environmental Protection Agency's (EPA) Office of Research and Development (ORD). Recently, version 5.1 of the CMAQ model (v5.1) was released to the public, incorporating a large number of science updates and extended capabilities over the previous release version of the model (v5.0.2). These updates include the following: improvements in the meteorological calculations in both CMAQ and the Weather Research and Forecast (WRF) model used to provide meteorological fields to CMAQ, updates to the gas and aerosol chemistry, revisions to the calculations of clouds and photolysis, and improvements to the dry and wet deposition in the model. Sensitivity simulations isolating several of the major updates to the modeling system show that changes to the meteorological calculations result in enhanced afternoon and early evening mixing in the model, periods when the model historically underestimates mixing. This enhanced mixing results in higher ozone (O3) mixing ratios on average due to reduced NO titration, and lower fine particulate matter (PM2.5) concentrations due to greater dilution of primary pollutants (e.g., elemental and organic carbon). Updates to the clouds and photolysis calculations greatly improve consistency between the WRF and CMAQ models and result in generally higher O3 mixing ratios, primarily due to reduced cloudiness and attenuation of photolysis in the model. Updates to the aerosol chemistry result in higher secondary organic aerosol (SOA) concentrations in the summer, thereby reducing summertime PM2.5 bias (PM2.5 is typically underestimated by CMAQ in the summer), while updates to the gas chemistry result in slightly higher O3 and PM2.5 on average in January and July. Overall, the seasonal variation in simulated PM2.5 generally improves in CMAQv5.1 (when considering all model updates), as simulated PM2.5 concentrations decrease in the winter (when PM2.5 is generally overestimated by CMAQ) and increase in the summer (when PM2.5 is generally underestimated by CMAQ). Ozone mixing ratios are higher on average with v5.1 vs. v5.0.2, resulting in higher O3 mean bias, as O3 tends to be overestimated by CMAQ throughout most of the year (especially at locations where the observed O3 is low); however, O3 correlation is largely improved with v5.1. Sensitivity simulations for several hypothetical emission reduction scenarios show that v5.1 tends to be slightly more responsive to reductions in NO x (NO + NO2), VOC and SO x (SO2 + SO4) emissions than v5.0.2, representing an improvement as previous studies have shown CMAQ to underestimate the observed reduction in O3 due to large, widespread reductions in observed emissions.

Predicting the effects of nanoscale cerium additives in diesel fuel on regional-scale air quality.

Diesel vehicles are a major source of air pollutant emissions. Fuel additives containing nanoparticulate cerium (nCe) are currently being used in some diesel vehicles to improve fuel efficiency. These fuel additives also reduce fine particulate matter (PM2.5) emissions and alter the emissions of carbon monoxide (CO), nitrogen oxides (NOx), and hydrocarbon (HC) species, including several hazardous air pollutants (HAPs). To predict their net effect on regional air quality, we review the emissions literature and develop a multipollutant inventory for a hypothetical scenario in which nCe additives are used in all on-road and nonroad diesel vehicles. We apply the Community Multiscale Air Quality (CMAQ) model to a domain covering the eastern U.S. for a summer and a winter period. Model calculations suggest modest decreases of average PM2.5 concentrations and relatively larger decreases in particulate elemental carbon. The nCe additives also have an effect on 8 h maximum ozone in summer. Variable effects on HAPs are predicted. The total U.S. emissions of fine-particulate cerium are estimated to increase 25-fold and result in elevated levels of airborne cerium (up to 22 ng/m3), which might adversely impact human health and the environment.

Diagnostic air quality model evaluation of source-specific primary and secondary fine particulate carbon.

Ambient measurements of 78 source-specific tracers of primary and secondary carbonaceous fine particulate matter collected at four midwestern United States locations over a full year (March 2004-February 2005) provided an unprecedented opportunity to diagnostically evaluate the results of a numerical air quality model. Previous analyses of these measurements demonstrated excellent mass closure for the variety of contributing sources. In this study, a carbon-apportionment version of the Community Multiscale Air Quality (CMAQ) model was used to track primary organic and elemental carbon emissions from 15 independent sources such as mobile sources and biomass burning in addition to four precursor-specific classes of secondary organic aerosol (SOA) originating from isoprene, terpenes, aromatics, and sesquiterpenes. Conversion of the source-resolved model output into organic tracer concentrations yielded a total of 2416 data pairs for comparison with observations. While emission source contributions to the total model bias varied by season and measurement location, the largest absolute bias of -0.55 µgC/m(3) was attributed to insufficient isoprene SOA in the summertime CMAQ simulation. Biomass combustion was responsible for the second largest summertime model bias (-0.46 µgC/m(3) on average). Several instances of compensating errors were also evident; model underpredictions in some sectors were masked by overpredictions in others.

Modeling the role of alkanes, polycyclic aromatic hydrocarbons, and their oligomers in secondary organic aerosol formation.

A computationally efficient method to treat secondary organic aerosol (SOA) from various length and structure alkanes as well as SOA from polycyclic aromatic hydrocarbons (PAHs) is implemented in the Community Multiscale Air Quality (CMAQ) model to predict aerosol concentrations over the United States. Oxidation of alkanes is predicted to produce more aerosol than oxidation of PAHs driven by relatively higher alkane emissions. SOA from alkanes and PAHs, although small in magnitude, can be a substantial fraction of the SOA from anthropogenic hydrocarbons, particularly in winter, and could contribute more if emission inventories lack intermediate volatility alkanes (>C(13)) or if the vehicle fleet shifts toward diesel-powered vehicles. The SOA produced from oxidation of alkanes correlates well with ozone and odd oxygen in many locations, but the lower correlation of anthropogenic oligomers with odd oxygen indicates that models may need additional photochemically dependent pathways to low-volatility SOA.

Model representation of secondary organic aerosol in CMAQv4.7.

Numerous scientific upgrades to the representation of secondary organic aerosol (SOA) are incorporated into the Community Multiscale Air Quality (CMAQ) modeling system. Additions include several recently identified SOA precursors: benzene, isoprene, and sesquiterpenes; and pathways: in-cloud oxidation of glyoxal and methylglyoxal, particle-phase oligomerization, and acid enhancement of isoprene SOA. NO(x)-dependent aromatic SOA yields are also added along with new empirical measurements of the enthalpies of vaporization and organic mass-to-carbon ratios. For the first time, these SOA precursors, pathways and empirical parameters are included simultaneously in an air quality model for an annual simulation spanning the continental U.S. Comparisons of CMAQ-modeled secondary organic carbon (OC(sec)) with semiempirical estimates screened from 165 routine monitoring sites across the U.S. indicate the new SOA module substantially improves model performance. The most notable improvement occurs in the central and southeastern U.S. where the regionally averaged temporal correlations (r) between modeled and semiempirical OC(sec) increase from 0.5 to 0.8 and 0.3 to 0.8, respectively, when the new SOA module is employed. Wintertime OC(sec) results improve in all regions of the continental U.S. and the seasonal and regional patterns of biogenic SOA are better represented.

To what extent can biogenic SOA be controlled?

The implicit assumption that biogenic secondary organic aerosol (SOA) is natural and can not be controlled hinders effective air quality management. Anthropogenic pollution facilitates transformation of naturally emitted volatile organic compounds (VOCs) to the particle phase, enhancing the ambient concentrations of biogenic secondary organic aerosol (SOA). It is therefore conceivable that some portion of ambient biogenic SOA can be removed by controlling emissions of anthropogenic pollutants. Direct measurement of the controllable fraction of biogenic SOA is not possible, but can be estimated through 3-dimensional photochemical air quality modeling. To examine this in detail, 22 CMAQ model simulations were conducted over the continental U.S. (August 15 to September 4, 2003). The relative contributions of five emitted pollution classes (i.e., NO(x), NH(3), SO(x), reactive non methane carbon (RNMC) and primary carbonaceous particulate matter (PCM)) on biogenic SOA were estimated by removing anthropogenic emissions of these pollutants, one at a time and all together. Model results demonstrate a strong influence of anthropogenic emissions on predicted biogenic SOA concentrations, suggesting more than 50% of biogenic SOA in the eastern U.S. can be controlled. Because biogenic SOA is substantially enhanced by controllable emissions, classification of SOA as biogenic or anthropogenic based solely on VOC origin is not sufficient to describe the controllable fraction.

Emissions inventory of PM2.5 trace elements across the United States.

This paper presents the first National Emissions Inventory (NEI) of fine particulate matter (PM2.5) that includes the full suite of PM2.5 trace elements (atomic number > 10) measured at ambient monitoring sites across the U.S. PM2.5 emissions in the NEI were organized and aggregated into a set of 84 source categories for which chemical speciation profiles are available (e.g., Unpaved Road Dust Agricultural Soil, Wildfires). Emission estimates for ten metals classified as Hazardous Air Pollutants (HAP) were refined using data from a recent HAP NEI. All emissions were spatially gridded, and U.S. emissions maps for dozens of trace elements (e.g., Fe, Ti) are presented for the first time. Nationally, the trace elements emitted in the highest quantities are silicon (3.8 x 10(5) ton/yr), aluminum (1.4 x 10(5) ton/yr), and calcium (1.3 x 10(5) ton/yr). Our chemical characterization of the PM2.5 inventory shows that most of the previously unspeciated emissions are comprised of crustal elements, potassium, sodium, chlorine, and metal-bound oxygen. This work also reveals that the largest PM2.5 sources lacking specific speciation data are off-road diesel-powered mobile equipment, road construction dust, marine vessels, gasoline-powered boats, and railroad locomotives.

Diagnostic model evaluation for carbonaceous PM2.5 using organic markers measured in the southeastern U.S.

Summertime concentrations of fine particulate carbon in the southeastern United States are consistently underestimated by air quality models. In an effort to understand the cause of this error, the Community Multiscale Air Quality model is instrumented to track primary organic and elemental carbon contributions from fifteen different source categories. The model results are speciated using published source profiles and compared with ambient measurements of 100 organic markers collected at eight sites in the Southeast during the 1999 summer. Results indicate that modeled contributions from vehicle exhaust and biomass combustion, the two largest sources of carbon in the emission inventory, are unbiased across the region. In Atlanta, good model performance for total carbon (TC) is attributed to compensating errors: overestimation of vehicle emissions with underestimations of other sources. In Birmingham, 35% of the TC underestimation can be explained by deficiencies in primary sources. Cigarette smoke and vegetative detritus are not in the inventory, but contribute less than 3% of the TC at each site. After the model results are adjusted for source-specific errors using the organic-marker measurements, an average of 1.6 microgC m(-3) remain unexplained. This corresponds to 26-38% of ambient TC concentrations at urban sites and up to 56% at rural sites. The most likely sources of unexplained carbon are discussed.