Development of PM_2.5 source impact spatial fields using a hybrid source apportionment air quality model

Abstract. An integral part of air quality management is knowledge of the impact of pollutant sources on ambient concentrations of particulate matter (PM). There is also a growing desire to directly use source impact estimates in health studies; however, source impacts cannot be directly measured. Several limitations are inherent in most source apportionment methods motivating the development of a novel hybrid approach that is used to estimate source impacts by combining the capabilities of receptor models (RMs) and chemical transport models (CTMs). The hybrid CTM–RM method calculates adjustment factors to refine the CTM-estimated impact of sources at monitoring sites using pollutant species observations and the results of CTM sensitivity analyses, though it does not directly generate spatial source impact fields. The CTM used here is the Community Multiscale Air Quality (CMAQ) model, and the RM approach is based on the chemical mass balance (CMB) model. This work presents a method that utilizes kriging to spatially interpolate source-specific impact adjustment factors to generate revised CTM source impact fields from the CTM–RM method results, and is applied for January 2004 over the continental United States. The kriging step is evaluated using data withholding and by comparing results to data from alternative networks. Data withholding also provides an estimate of method uncertainty. Directly applied (hybrid, HYB) and spatially interpolated (spatial hybrid, SH) hybrid adjustment factors at withheld observation sites had a correlation coefficient of 0.89, a linear regression slope of 0.83 ± 0.02, and an intercept of 0.14 ± 0.02. Refined source contributions reflect current knowledge of PM emissions (e.g., significant differences in biomass burning impact fields). Concentrations of 19 species and total PM_2.5 mass were reconstructed for withheld observation sites using HYB and SH adjustment factors. The mean concentrations of total PM_2.5 at withheld observation sites were 11.7 (± 8.3), 16.3 (± 11), 8.59 (± 4.7), and 9.2 (± 5.7) μg m⁻³ for the observations, CTM, HYB, and SH predictions, respectively. Correlations improved for concentrations of major ions, including nitrate (CMAQ–DDM (decoupled direct method): 0.404, SH: 0.449), ammonium (CMAQ–DDM: 0.454, SH: 0.492), and sulfate (CMAQ–DDM: 0.706, SH: 0.730). Errors in simulated concentrations of metals were reduced considerably: 295 % (CMAQ–DDM) to 139 % (SH) for vanadium; and 1340 % (CMAQ–DDM) to 326 % (SH) for manganese. Errors in simulated concentrations of some metals are expected to remain given the uncertainties in source profiles. Species concentrations were reconstructed using SH results, and the error relative to observed concentrations was greatly reduced as compared to CTM-simulated concentrations. Results demonstrate that the hybrid method along with a spatial extension can be used for large-scale, spatially resolved source apportionment studies where observational data are spatially and temporally limited.