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Source apportionment analysis was conducted with positive matrixfactorization (PMF) and principal component analysis (PCA) methods usingconcentrations of speciated mercury (Hg), i.e., gaseous elemental mercury(GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM),and other air pollutants collected at Kejimkujik National Park, Nova Scotia,Canada, in 2009 and 2010. The results were largely consistent between the 2 years for both methods. The same four source factors were identified in eachyear using PMF method. In both years,  factor photochemistry and re-emissionhad the largest contributions to atmospheric Hg, while the contributions ofcombustion emission and industrial sulfur varied slightly between the 2 years. Four components were extracted with air pollutants only in each yearusing PCA method. Consistencies between the results of PMF and PCA include(1) most or all PMF factors overlapped with PCA components, (2) both methodssuggest strong impact of photochemistry but little association betweenambient Hg and sea salt, and (3) shifting of PMF source profiles and sourcecontributions from one year to another was echoed in PCA. Inclusion ofmeteorological parameters led to identification of an additional component,Hg wet deposition in PCA, while it did not affect the identification ofother components.  The PMF model performance was comparable in 2009 and 2010. Among the threeHg forms, the agreements between model-reproduced and observed annual meanconcentrations were excellent for GEM, very good for PBM, and acceptable forGOM. However, on a daily basis, the agreement was very good for GEM but poorfor GOM and PBM. Sensitivity tests suggest that increasing sample size byimputation is not effective in improving model performance, while reducingthe fraction of concentrations below method detection limit, by eitherscaling GOM and PBM to higher concentrations or combining them to reactivemercury, is effective. Most of the data treatment options considered hadlittle impact on the source identification or contribution

atmospheric chemistry and physics

Potential sources and processes affecting speciated atmospheric mercury at Kejimkujik National Park, Canada: comparison of receptor models and data treatment methods