Sivaraman Balachandran

Bayesian-based ensemble source apportionment of PM2.5.

A Bayesian source apportionment (SA) method is developed to provide source impact estimates and associated uncertainties. Bayesian-based ensemble averaging of multiple models provides new source profiles for use in a chemical mass balance (CMB) SA of fine particulate matter (PM2.5). The approach estimates source impacts and their uncertainties by using a short-term application of four individual SA methods: three receptor-based models and one chemical transport model. The method is used to estimate two seasonal distributions of source profiles that are used in SA for a long-term PM2.5 data set. For each day in a long-term PM2.5 data set, 10 source profiles are sampled from these distributions and used in a CMB application, resulting in 10 SA results for each day. This formulation results in a distribution of daily source impacts rather than a single value. The average and standard deviation of the distribution are used as the final estimate of source impact and a measure of uncertainty, respectively. The Bayesian-based source impacts for biomass burning correlate better with observed levoglucosan (R(2) = 0.66) and water-soluble potassium (R(2) = 0.63) than source impacts estimated using more traditional methods and more closely agrees with observed total mass. The Bayesian approach also captures the expected seasonal variation of biomass burning and secondary impacts and results in fewer days with sources having zero impact. Sensitivity analysis found that using non-informative prior weighting performed better than using weighting based on method-derived uncertainties. This approach can be applied to long-term data sets from speciation network sites of the United States Environmental Protection Agency (U.S. EPA). In addition to providing results that are more consistent with independent observations and known emission sources being present, the distributions of source impacts can be used in epidemiologic analyses to estimate uncertainties associated with the SA results.

Development of outcome-based, multipollutant mobile source indicators.

Multipollutant indicators of mobile source impacts are developed from readily available CO, NOx, and elemental carbon (EC) data for use in air quality and epidemiologic analysis. Two types of outcome-based Integrated Mobile Source Indicators (IMSI) are assessed. The first is derived from analysis of emissions of EC, CO, and NOx such that pollutant concentrations are mixed and weighted based on emission ratios for both gasoline and diesel vehicles. The emission-based indicators (IMSIEB) capture the impact of mobile sources on air quality estimated from receptor models and their uncertainty is comparable to measurement and source apportionment uncertainties. The IMSIEB have larger correlation between two different receptor sites impacted by traffic than single pollutants, suggesting they are better indicators of the local impact of mobile sources. A sensitivity analysis of fractions of pollutants in a two-pollutant mixture and the inclusion in an epidemiologic model is conducted to develop a second set of indicators based on health outcomes. The health-based indicators (IMSIHB) are weighted combinations of CO, NOx, and EC pairs that have the lowest P value in their association with cardiovascular disease emergency department visits, possibly due to their better spatial representativeness. These outcome-based, multipollutant indicators can provide support for the setting of multipollutant air quality standards and other air quality management activities. Implications: Integrated mobile source indicators (IMSI) were developed and assessed for use in air quality and epidemiologic analysis. IMSI contribute to fill the gap in the path towards a multipollutant air quality approach in two aspects: IMSI represent an innovative way to identify mixtures of pollutants based on outcomes and constitutes an alternative approach to assess multipollutant health effects. IMSI developed for mobile sources can be easily applied to other sources. Results can support the setting of multipollutant air quality standards. Supplemental Material Supplemental materials are available for this article. Go to the publishers online edition of the Journal of the Air & Waste Management Association for materials showing the estimation of uncertainties using propagation of errors, comparison of source impacts from CMB and PMF and wind direction and speed for the Jefferson Street monitoring location in Atlanta.

Ensemble-Based Source Apportionment of Fine Particulate Matter and Emergency Department Visits for Pediatric Asthma

Epidemiologic studies utilizing source apportionment (SA) of fine particulate matter have shown that particles from certain sources might be more detrimental to health than others; however, it is difficult to quantify the uncertainty associated with a given SA approach. In the present study, we examined associations between source contributions of fine particulate matter and emergency department visits for pediatric asthma in Atlanta, Georgia (2002-2010) using a novel ensemble-based SA technique. Six daily source contributions from 4 SA approaches were combined into an ensemble source contribution. To better account for exposure uncertainty, 10 source profiles were sampled from their posterior distributions, resulting in 10 time series with daily SA concentrations. For each of these time series, Poisson generalized linear models with varying lag structures were used to estimate the health associations for the 6 sources. The rate ratios for the source-specific health associations from the 10 imputed source contribution time series were combined, resulting in health associations with inflated confidence intervals to better account for exposure uncertainty. Adverse associations with pediatric asthma were observed for 8-day exposure to particles generated from diesel-fueled vehicles (rate ratio = 1.06, 95% confidence interval: 1.01, 1.10) and gasoline-fueled vehicles (rate ratio = 1.10, 95% confidence interval: 1.04, 1.17).

Application of an ensemble-trained source apportionment approach at a site impacted by multiple point sources.

Four receptor models and a chemical transport model were used to quantify PM2.5 source impacts at the St. Louis Supersite (STL-SS) between June 2001 and May 2003. The receptor models used two semi-independent data sets, with the first including ions and trace elements and the second including 1-in-6 day particle-bound organics. Since each source apportionment (SA) technique has limitations, this work compares results from the five different SA approaches to better understand the biases and limitations of each. The source impacts calculated by these models were then integrated into a constrained, ensemble-trained SA approach. The ensemble method offers several improvements over the five individual SA techniques at the STL-SS. Primarily, the ensemble method calculates source impacts on days when individual models either do not converge to a solution or do not have adequate input data to develop source impact estimates. When compared with a chemical mass balance approach using measurement-based source profiles, the ensemble method improves fit statistics, reducing chi-squared values and improving PM2.5 mass reconstruction. Compared to other receptor models, the ensemble method also calculates zero or negative impacts from major emissions sources (e.g., secondary organic carbon (SOC) and diesel vehicles) for fewer days. One limitation of this analysis was that a composite metals profile was used in the ensemble analysis. Although STL-SS is impacted by multiple metals processing point sources, several of the initial SA methods could not resolve individual metals processing impacts. The results of this analysis also reveal some of the subjectivities associated with applying specific SA models at the STL-SS. For instance, Positive Matrix Factorization results are very sensitive to both the fitting species and number of factors selected by the user. Conversely, Chemical Mass Balance results are sensitive to the source profiles used to represent local metals processing emissions. Additionally, the different SA approaches predict different impacts for the same source on a given day, with correlation coefficients ranging from 0.034 to 0.65 for gasoline vehicles, -0.54-0.48 for diesel vehicles, -0.29-0.81 for dust, -0.34-0.89 for biomass burning, 0.38-0.49 for metals processing, and -0.25-0.51 for SOC. These issues emphasize the value of using several different SA techniques at a given receptor site, either by comparing source impacts predicted by different models or by using an ensemble-based technique.

Associations between Source-Specific Fine Particulate Matter and Emergency Department Visits for Respiratory Disease in Four U.S. Cities.

Background: Short-term exposure to ambient fine particulate matter (PM2.5) concentrations has been associated with increased mortality and morbidity. Determining which sources of PM2.5 are most toxic can help guide targeted reduction of PM2.5. However, conducting multicity epidemiologic studies of sources is difficult because source-specific PM2.5 is not directly measured, and source chemical compositions can vary between cities. Objectives: We determined how the chemical composition of primary ambient PM2.5 sources varies across cities. We estimated associations between source-specific PM2.5 and respiratory disease emergency department (ED) visits and examined between-city heterogeneity in estimated associations. Methods: We used source apportionment to estimate daily concentrations of primary source-specific PM2.5 for four U.S. cities. For sources with similar chemical compositions between cities, we applied Poisson time-series regression models to estimate associations between source-specific PM2.5 and respiratory disease ED visits. Results: We found that PM2.5 from biomass burning, diesel vehicle, gasoline vehicle, and dust sources was similar in chemical composition between cities, but PM2.5 from coal combustion and metal sources varied across cities. We found some evidence of positive associations of respiratory disease ED visits with biomass burning PM2.5; associations with diesel and gasoline PM2.5 were frequently imprecise or consistent with the null. We found little evidence of associations with dust PM2.5. Conclusions: We introduced an approach for comparing the chemical compositions of PM2.5 sources across cities and conducted one of the first multicity studies of source-specific PM2.5 and ED visits. Across four U.S. cities, among the primary PM2.5 sources assessed, biomass burning PM2.5 was most strongly associated with respiratory health. Citation: Krall JR, Mulholland JA, Russell AG, Balachandran S, Winquist A, Tolbert PE, Waller LA, Sarnat SE. 2017. Associations between source-specific fine particulate matter and emergency department visits for respiratory disease in four U.S. cities. Environ Health Perspect 125:97–103; http://dx.doi.org/10.1289/EHP271

Development of PM2.5 source profiles using a hybrid chemical transport-receptor modeling approach

Laboratory-based or in situ PM2.5 source profiles may not represent the pollutant composition for the sources in a different study location due to spatially and temporally varying characteristics, such as fuel or crustal element composition, or due to differences in emissions behavior under ambient versus laboratory conditions. In this work, PM2.5 source profiles were estimated for 20 sources using a novel optimization approach that incorporates observed concentrations with source impacts from a chemical transport model (CTM) to capture local pollutant characteristics. Nonlinear optimization was used to minimize the error between source profiles, CTM source impacts, and observations. In a 2006 U.S. application, spatial and seasonal variability was seen for coal combustion, dust, fires, metals processing, and other source profiles when compared to the reference profiles, with variability in species fractions over 400% (calcium in dust) compared to mean contributions of the same species. Revised profiles improved the spatial and temporal bias in modeled concentrations of several trace metal species, including Na, Al, Ca, Mn, Cu, As, Se, Br, and Pb. In an application of the CMB-iteration model for two U.S. cities, revised profiles estimated higher biomass burning and dust impacts for summer compared with previous studies. Source profile optimization can be useful for source apportionment studies that have limited availability of source profile data for the location of interest.

Improved Spatiotemporal Source-Based Air Pollutant Mixture Characterization for Health Studies

The growing availability of spatially resolved health data sets (i.e., resident and county level patient records) requires spatially resolved exposure or air quality metrics to investigate the impact of air pollution on health outcomes. While daily air quality data are essential in time-series epidemiologic analysis, the spatial distribution of the observations is limited. Air pollution modeling (i.e., chemical transport modeling (CTM)) addresses this by producing spatially resolved air quality predictions using terrain, emissions and meteorology inputs. However, predicted concentrations may be biased. This work incorporates unique data fusion approaches to combine air quality observations from regulatory monitoring networks (OBS) with the output from a CTM (CMAQ) to generate spatially and temporally resolved gaseous and PM species concentrations. Species concentrations alone cannot directly identify emission sources or characterize pollutant mixtures, therefore source apportionment (SA) models are required to estimate source impacts. The focus of this work is a comparison of SA results for three U.S. regions with differing air pollution sources, St. Louis, Missouri; Atlanta, Georgia; and Dallas-Fort Worth, Texas.