Seasonal and spatial patterns of mercury wet deposition in the United States: Constraints on the contribution from North American anthropogenic sources

Observed wet deposition fluxes of mercury in the United States show a maximum in the Southeast, and a consistent seasonal variation (maximum in summer, minimum in winter) that increases in amplitude from north to south. We simulate these patterns successfully with a global 3-D chemical transport model (GEOS-Chem) including our best estimates of sources and processes. We attribute the high wet deposition over the Southeast in summer to scavenging of upper-altitude Hg(II) by deep convection. Seasonal variation at higher latitudes is attributed to a combination of enhanced summertime oxidation of Hg(0) and inefficient scavenging of Hg(II) by snow. Scavenging of Hg(II) from above the boundary layer contributes over half of wet deposition to the US in the model. Even within the boundary layer, we find that most of Hg(II) originates from the global mercury pool. Wet deposition in the model accounts for only 30% of total mercury deposition in the US, the remainder being from dry deposition, including 42% from Hg(0) uptake. North American anthropogenic emissions contribute 20% of total mercury deposition in the US (up to 50% in the industrial Midwest and Northeast). (C) 2008 Elsevier Ltd. All rights reserved.