Assessing the Emission Sources of Atmospheric Mercury in Wet Deposition Across Illinois, USA

Abstract

From August 2007 to August 2009, we collected event-based precipitation samples for mercury (Hg) and trace element analysis at four sites in Illinois, USA. The objectives of these measurements were to quantify the levels of Hg wet deposition across the state, and to assess the contributions to Hg in precipitation from major local and regional emission sources. The measurement sites were located in Chicago, Peoria, Nilwood, and Carbondale, IL. We were not able to identify a clear spatial gradient in Hg wet deposition among the sites. At all four locations we frequently observed Hg concentrations in precipitation > 25 ng/L, while each site received > 10 μg/m2 of Hg wet deposition annually, suggesting a substantial impact from local and regional anthropogenic emission sources. We applied the multivariate statistical receptor model Positive Matrix Factorization (PMF) to the measured Hg and trace element wet deposition amounts at the four sites. The results suggested that 60-83% of total Hg deposition at each site could be attributed to coal combustion emissions. Although we identified other source signatures in the precipitation composition, including cement manufacturing, metal smelting / waste incineration, and iron-steel production, these sources contributed substantially less to the measured amounts of Hg wet deposition. We also applied the hybrid receptor model Quantitative Transport Bias Analysis (QTBA) to the Hg wet deposition data from each site to identify the major source regions associated with the measured values. Results suggested that sources in the Chicago/Gary, St. Louis, and Ohio River Valley urban/industrial areas had a substantial impact on Hg wet deposition, strongly supporting the conclusion that local and regional coal combustion was the largest source of Hg wet deposition in Illinois.