Assessing the emission sources of atmospheric mercury in wet deposition across Illinois

From August 4, 2007 to August 31, 2009, we collected event-based precipitation samples for mercury (Hg) and trace element analyses at four sites in Illinois (IL), USA. The objectives of these measurements were to quantify Hg wet deposition across the state, and to assess the contributions to Hg in precipitation from major local and regional emission sources. Monitoring sites were located, from north to south, in Chicago, Peoria, Nilwood, and Carbondale, IL. Measurements from these four sites demonstrated that a clear spatial gradient in Hg wet deposition was not evident across the state. Each site received>10μgm(-2) of Hg wet deposition annually, and these observed values were comparable to annual Hg wet deposition measurements from other event-based precipitation monitoring sites in source-impacted areas of the Midwestern U.S. We applied the multivariate statistical receptor model, Positive Matrix Factorization (EPA PMF v3.0), to the measured Hg and trace element wet deposition amounts at the four sites. Results suggested that 50% to 74% of total Hg wet deposition at each site could be attributed to coal combustion emissions. The other source signatures identified in the precipitation compositions included cement manufacturing, mixed metal smelting/waste incineration, iron-steel production, and a phosphorus source. We also applied a hybrid receptor model, Quantitative Transport Bias Analysis (QTBA), to the Hg wet deposition datasets to identify the major source regions associated with the measured values. The calculated QTBA probability fields suggested that transport from urban/industrial areas, such as Chicago/Gary, St. Louis, and the Ohio River Valley, resulted in some of the highest estimated event-based Hg wet deposition amounts at the four sites (potential mass transfer of up to 0.32μgm(-2)). The combined application of PMF and QTBA supported the hypothesis that local and regional coal combustion was the largest source of Hg wet deposition in Illinois.