Assessing the atmospheric deposition of mercury to Lake Michigan: The importance of the Chicago/Gary urban area on wet and dry deposition.

Abstract

Mercury is a toxic bioaccumulative substance found in aquatic ecosystems. The results of the first study of atmospheric mercury deposition into Lake Michigan and the relative importance of the Chicago/Gary urban area were investigated as part of the Lake Michigan Mass Balance Study (LMMBS) and the Atmospheric Exchange Over Lakes and Oceans Study (AEOLOS). Event wet-only precipitation, total aerosol, and vapor phase samples were collected for mercury and trace element determinations from five sites around Lake Michigan from July 1994 through October 1995 as part of the LMMBS. In addition, intensive over-water measurements were conducted aboard the EPA research vessel Lake Guardian during the summer of 1994 and the winter of 1995 as part of the AEOLOS. Atmospheric mercury concentrations were from two to ten times higher in the Chicago/Gary urban area. Wet and dry Hg deposition (including reactive gaseous Hg) were calculated to Lake Michigan using a hybrid receptor modeling framework. The model utilized mercury monitoring data collected during the LMMBS and AEOLOS together with high resolution over-water meteorological data provided by the National Oceanic and Atmospheric Administration. Atmospheric deposition was found to be the primary pathway for mercury input to Lake Michigan, contributing approximately 84% of the estimated 1419 Kg annual flux. Wet deposition (10.6 $\mu$g m$\sp{-2})$ and dry deposition (10.0 $\mu$g m$\sp{-2})$ contributed almost equally to the annual atmospheric Hg deposition of 20.6 $\mu$g m$\sp{-2}$ (1189 Kg). A strong urban influence was observed in the over-water mercury deposition estimates in the southern portion of the lake. An independent meteorological transport analysis determined that local sources in the Chicago/Gary urban area significantly impacted the LMMBS sites around Lake Michigan. The Chicago/Gary urban area was found to contribute about 20% (127 Kg) of the annual atmospheric mercury deposition to Lake Michigan. Multivariate statistical analysis of measurements in Chicago identified coal combustion, incineration, steel production, and cement production as the major sources of Hg contributing to the enhanced atmospheric mercury deposition to the lake. The magnitude of local anthropogenic mercury sources in the Chicago/Gary urban area suggest that emission reductions would effectively reduce atmospheric mercury deposition into Lake Michigan.