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.

Trends in Chemical Composition of Global and Regional Population-Weighted Fine Particulate Matter Estimated for 25 Years.

We interpret in situ and satellite observations with a chemical transport model (GEOS-Chem, downscaled to 0.1° × 0.1°) to understand global trends in population-weighted mean chemical composition of fine particulate matter (PM2.5). Trends in observed and simulated population-weighted mean PM2.5 composition over 1989-2013 are highly consistent for PM2.5 (-2.4 vs -2.4%/yr), secondary inorganic aerosols (-4.3 vs -4.1%/yr), organic aerosols (OA, -3.6 vs -3.0%/yr) and black carbon (-4.3 vs -3.9%/yr) over North America, as well as for sulfate (-4.7 vs -5.8%/yr) over Europe. Simulated trends over 1998-2013 also have overlapping 95% confidence intervals with satellite-derived trends in population-weighted mean PM2.5 for 20 of 21 global regions. Over 1989-2013, most (79%) of the simulated increase in global population-weighted mean PM2.5 of 0.28 µg m-3yr-1 is explained by significantly (p < 0.05) increasing OA (0.10 µg m-3yr-1), nitrate (0.05 µg m-3yr-1), sulfate (0.04 µg m-3yr-1), and ammonium (0.03 µg m-3yr-1). These four components predominantly drive trends in population-weighted mean PM2.5 over populous regions of South Asia (0.94 µg m-3yr-1), East Asia (0.66 µg m-3yr-1), Western Europe (-0.47 µg m-3yr-1), and North America (-0.32 µg m-3yr-1). Trends in area-weighted mean and population-weighted mean PM2.5 composition differ significantly.

Ozone trends across the United States over a period of decreasing NOx and VOC emissions.

In this work, we evaluate ambient ozone trends at urban, suburban, and rural monitoring sites across the United States over a period of decreasing NOx and VOC emissions (1998-2013). We find that decreasing ozone trends generally occur in the summer, in less urbanized areas, and at the upper end of the ozone distribution. Conversely, increasing ozone trends generally occur in the winter, in more urbanized areas, and at the lower end of the ozone distribution. The 95(th) percentile ozone concentrations decreased at urban, suburban, and rural monitors by 1-2 ppb/yr in the summer and 0.5-1 ppb/yr in the winter. In the summer, there are both increasing and decreasing trends in fifth percentile ozone concentrations of less than 0.5 ppb/yr at urban and suburban monitors, while fifth percentile ozone concentrations at rural monitors decreased by up to 1 ppb/yr. In the winter, fifth percentile ozone concentrations generally increased by 0.1-1 ppb/yr. These results demonstrate the large scale success of U.S. control strategies targeted at decreasing peak ozone concentrations. In addition, they indicate that as anthropogenic NOx emissions have decreased, the ozone distribution has been compressed, leading to less spatial and temporal variability.

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.

Receptor modeling of ambient particulate matter data using positive matrix factorization: review of existing methods.

Methods for apportioning sources of ambient particulate matter (PM) using the positive matrix factorization (PMF) algorithm are reviewed. Numerous procedural decisions must be made and algorithmic parameters selected when analyzing PM data with PMF. However, few publications document enough of these details for readers to evaluate, reproduce, or compare results between different studies. For example, few studies document why some species were used and others not used in the modeling, how the number of factors was selected, or how much uncertainty exists in the solutions. More thorough documentation will aid the development of standard protocols for analyzing PM data with PMF and will reveal more clearly where research is needed to help future analysts select from the various possible procedures and parameters available in PMF. For example, research likely is needed to determine optimal approaches for handling data below detection limits, ways to apportion PM mass among sources identified by PMF, and ways to estimate uncertainties in the solution. The review closes with recommendations for documenting the methodological details of future PMF analyses.

Relationships of Indoor, Outdoor, and Personal Air (RIOPA). Part I. Collection methods and descriptive analyses.

This study on the relationships of indoor, outdoor, and personal air (RIOPA) was undertaken to collect data for use in evaluating the contribution of outdoor sources of air toxics and particulate matter (PM) to personal exposure. The study was not designed to obtain a population-based sample, but rather to provide matched indoor, outdoor, and personal concentrations in homes that varied in their proximity to outdoor pollution sources and had a wide range of air exchange rates (AERs). This design allowed examination of relations among indoor, outdoor, and personal concentrations of air toxics and PM across a wide range of environmental conditions; the resulting data set obtained for a wide range of environmental pollutants and AERs can be used to evaluate exposure models. Approximately 100 households with residents who do not smoke participated in each of three cities in distinct locations expected to have different climates and housing characteristics: Elizabeth, New Jersey; Houston, Texas; and Los Angeles County, California. Questionnaires were administered to characterize homes, neighborhoods, and personal activities that might affect exposures. The concentrations of a suite of volatile organic compounds (VOCs) and carbonyl compounds, as well as the fraction of airborne particulate matter with a mass median aerodynamic diameter < or = 2.5 microm (PM2.5), were measured during continuous 48-hour sessions in which indoor, outdoor, and personal air samples were collected simultaneously. During the same 48-hour period, the AER (exchanges/hr; x hr(-1)) was determined in each home, and carbonyl compounds were measured inside vehicle cabins driven by a subset of the participants. In most of the homes, measurements were made twice, during two different seasons, to obtain a wide distribution of AERs. This report presents in detail the data collection methods, quality control measures, and initial analyses of data distributions and relations among indoor, outdoor, and personal concentrations. The results show that indoor sources dominated personal and indoor air concentrations of many measured VOCs and carbonyl compounds. For several measured species, personal concentrations were higher than either indoor or outdoor concentrations, indicating the presence of some sources closely related to personal activities. For some species there were no significant indoor sources in the majority of the homes; thus indoor concentrations were mainly determined by outdoor concentrations in these homes. The range of distributions of air concentrations for the measured VOCs, formaldehyde and acetaldehyde, PM2.5, and AERs were generally consistent with values reported previously in the literature. Thus associations derived from or models based on this data set that may link the influence of outdoor sources with indoor air concentrations of air toxics and PM2.5 can be relevant to other urban settings. The simultaneous measurements of indoor concentrations, outdoor concentrations, AERs, and room volumes allowed the use of a mass balance model, under the steady-state approximation, to mechanistically examine the relative contributions of indoor and outdoor sources to measured indoor concentrations on a home-by-home basis. Estimated indoor source strengths for VOCs and carbonyl compounds varied widely from home to home, consistent with the indoor-outdoor concentration patterns, as shown in scatter plots. The indoor source estimations agreed with published values for PM2.5 and with the general understanding of sources of VOCs and carbonyl compounds. The source strengths reported here, derived from hundreds of homes, are an important contribution to the literature on exposure to air toxics. For the first time for many compounds, these estimates present a cohesive set of measurements across a range of air toxics in paired indoor, outdoor, and personal samples along with AER and questionnaire results that can be used for future analyses of indoor air quality. The estimation of outdoor contributions to measured indoor concentrations provides insights about the relative importance of indoor and outdoor sources in determining indoor concentrations, the main determinant of personal exposure for most of the measured compounds. In this report simple statistical tests mainly of the pooled data were used to analyze differences by sampling site, emission source type, season, home type, and home age. Paired adult-child personal concentrations within the same home were also compared using the pooled data set. These analyses generated some intriguing results that warrant more in-depth investigation in the future.