Identification of atmospheric mercury sources and transport pathways on local and regional sales.

摘要

Mercury (Hg) is a hazardous air pollutant and bioaccumulative neurotoxin whose intricate atmospheric chemistry complicates our ability to define Hg source-receptor relationships on all scales. Our detailed measurements of Hg in its different forms together with atmospheric tracers have improved our understanding of Hg chemistry and transport. Daily-event precipitation samples collected from 1995 to 2006 in Underhill, VT were examined to identify Hg wet deposition trends and source influences. Analysis revealed that annual Hg deposition at this fairly remote location did not vary significantly over the 12-year period. While a decreasing trend in volume-weighted mean Hg concentration was observed, Hg wet deposition did not decline as transport of emissions from the Midwest and along the Atlantic Coast consistently contributed to the largest observed Hg wet deposition events. Receptor modeling of Hg and trace elements in precipitation indicated that ---60% of Hg wet deposition at Underhill could be attributed to emissions from coal-fired utility boilers (CFUBs), and their contribution to Hg wet deposition did not change significantly over time. Hybrid-receptor modeling further defined these CFUBs to be located predominantly in the Midwestern U.S.;Atmospheric Hg chemistry and transport from the Chicago urban/industrial area was the focus of speciated Hg measurements performed in the southern Lake Michigan basin during summer 2007. Transport from Chicago, IL to Holland, MI occurred during 27% of the study period, resulting in a five-fold increase in divalent reactive gaseous Hg (RGM) at the downwind Holland site. Dispersion modeling of case study periods demonstrated that under southwesterly flow approximately half of the RGM in Holland could be attributed to primary RGM emissions from Chicago after transport and dispersion, with the remainder due to Hg0 oxidation in the atmosphere en route. Precipitation and ambient vapor phase samples were also collected in Chicago, Holland, and Dexter, MI and analyzed for Hg isotopes. The Hg isotopic fractionation observed in atmospheric samples was in contrast to a recently published report which predicted that aqueous photoreduction may be a dominant source of atmospheric Hg. Our results suggest that other redox reactions and source related processes likely contribute to isotopic fractionation of atmospheric Hg.