Hyper-local to regional exposure contrast of source-resolved PM2.5 components across the contiguous United States: implications for health assessment

Background: Improved understanding of sources and processes that drive exposure contrast of fine particulate matter (PM2.5) is essential for designing and interpreting epidemiological study outcomes. Objective: We investigate the contribution of various sources and processes to PM2.5 exposure contrasts at different spatial scales across the continental United States. Methods: We consider three cases: exposure contrast within a metro area, nationwide exposure contrast with high spatial resolution, and nationwide exposure contrast with low spatial resolution. Using national empirical model estimates of source- and chemically specific PM2.5 concentration predictions, we quantified the contribution of various sources and processes to PM2.5 exposure contrasts in these three cases. Results: At the metro level (i.e., metropolitan statistical area; MSA), exposure contrasts of PM2.5 vary between -1.8 to 1.4 mu g m(-3) relative to the MSA-mean with about 50% of within-MSA exposure contrast of PM2.5 caused by cooking and mobile source primary PM2.5. For the national exposure contrast at low-resolution (i.e., using MSA-average mean concentrations), exposure contrasts (relative to the national mean: -3.9 to 3.2 mu g m(-3)) are larger than within an MSA with similar to 80% of the variation due to secondaryPM2.5. National exposure contrast at high resolution (census block) has the largest absolute range (relative to the national mean: -4.7 to 3.7 mu g m-3) due to both regional and intra-urban contributions; on average, 65% of the national exposure contrast is due to secondary PM2.5 with the remaining from the primary PM2.5 (cooking and mobile source 26%, other 9%). Impact: Our study provides a comprehensive analysis of the sources and processes that contribute to exposure contrasts of PM2.5 across different geographic areas in the US. For the first time on a national scale, we used high spatial resolution source-specific exposure estimates to identify the primary contributors to PM2.5 exposure contrasts. The study also highlights the advantages of different study designs for investigating the health impacts of specific PM2.5 components. The findings provide novel insights that can inform public health policies aimed at reducing PM2.5 exposure and advance the understanding of the epidemiological study outcomes.