Fine Particle Iron in Soils and Road Dust Is Modulated by Coal-Fired Power Plant Sulfur

Transition metal ions, such as water-soluble iron (WS-Fe), are toxic components of fine particles (PM_2.5). In Atlanta, from 1998 to 2013, a previous study found that WS-Fe was the PM_2.5 species most associated with adverse cardiovascular outcomes. We examined this data set to investigate the sources of WS-Fe and the effects of air quality regulations on ambient levels of WS-Fe. We find that insoluble forms of iron in mineral and road dust combined with sulfate from coal-fired electrical generating units were converted into soluble forms by sulfate-driven acid dissolution. Sulfate produced both the highly acidic aerosol (summer pH 1.5-2) and liquid water required for the aqueous phase acid dissolution, but variability in WS-Fe was mainly driven by particle liquid water. These processes were more pronounced in summer when particles were most acidic, whereas in winter the relative importance of WS-Fe from combustion emissions increased. Although WS-Fe constituted a minute fraction of PM_2.5 mass (0.15%), the WS-Fe-PM_2.5 mass correlation was high (r = 0.67) and may be explained by these formation routes, which, in part, could account for observed associations between PM_2.5 mass and adverse health seen in past studies. Similar processes are expected in many regions, implying that these unexpected benefits from coal-burning reduction may be widespread.