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Atmospheric deposition is a significant loading pathway for polychlorinated dibenzo-p-dioxins and dibenzofurans (dioxin) to the Great Lakes. An innovative approach using NOAA's HYSPLIT atmospheric fate and transport model was developed to estimate the 1996 dioxin contribution to each lake from each of 5,700 point sources and 42,600 area sources in a U.S./Canadian air emissions inventory. These unusually detailed source-receptor modeling results show that deposition to each lake arises from a broad geographical region, with significant contributions from up to 2,000 km away. The source categories contributing most significantly to 1996 dioxin deposition appear to be municipal waste incineration, iron sintering, medical waste incineration, and cement kilns burning hazardous waste. Model-predicted air concentrations and deposition fluxes were consistent with ambient measurement data, within the uncertainties in each, but there may be a moderate tendency toward underestimation using midrange emissions estimates. The most likely reason for this tendency appears to be missing or underestimated emissions sources, but in-situ atmospheric formation of octachlorinated dibenzo-p-dioxin (OCDD) and heptachlorinated dibenzo-p-dioxin (HpCDD) may have also contributed. Despite uncertainties, the findings regarding the relative importance of different sources types and source regions appear to be relatively robust and may be useful in prioritizing pollution prevention efforts.

Mercury contamination in the Great Lakes continues to have important public health and wildlife ecotoxicology impacts, and atmospheric deposition is a significant ongoing loading pathway. The objective of this study was to estimate the amount and source-attribution for atmospheric mercury deposition to each lake, information needed to prioritize amelioration efforts. A new global, Eulerian version of the HYSPLIT-Hg model was used to simulate the 2005 global atmospheric transport and deposition of mercury to the Great Lakes. In addition to the base case, 10 alternative model configurations were used to examine sensitivity to uncertainties in atmospheric mercury chemistry and surface exchange. A novel atmospheric lifetime analysis was used to characterize fate and transport processes within the model. Model-estimated wet deposition and atmospheric concentrations of gaseous elemental mercury (Hg(0)) were generally within ∼10% of measurements in the Great Lakes region. The model overestimated non-Hg(0) concentrations by a factor of 2-3, similar to other modeling studies. Potential reasons for this disagreement include model inaccuracies, differences in atmospheric Hg fractions being compared, and the measurements being biased low. Lake Erie, downwind of significant local/regional emissions sources, was estimated by the model to be the most impacted by direct anthropogenic emissions (58% of the base case total deposition), while Lake Superior, with the fewest upwind local/regional sources, was the least impacted (27%). The U.S. was the largest national contributor, followed by China, contributing 25% and 6%, respectively, on average, for the Great Lakes. The contribution of U.S. direct anthropogenic emissions to total mercury deposition varied between 46% for the base case (with a range of 24-51% over all model configurations) for Lake Erie and 11% (range 6-13%) for Lake Superior. These results illustrate the importance of atmospheric chemistry, as well as emissions strength, speciation, and proximity, to the amount and source-attribution of mercury deposition.

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The movement of excess reactive nitrogen (N r ) from anthropogenic activities to natural ecosystems has been described as one of the most serious environmental threats facing modern society. One of the approaches for tracking this movement is the use of budgets that quantify fluxes. We constructed an N r budget for Canada using measured and modeled values from the scientific literature, government databases, and data from new agri-environmental indicators, in order to produce information for policy makers and scientists to understand the major flows of nitrogen to allow a better assessment of risks to the Canadian environment. We divided the Canadian territory south of 60°N into areas dominated by natural ecosystems, as well as by agricultural and urban/industrial activities to evaluate N r flows within, between, and out of these units. We show that Canada is a major exporter of N r due to the availability of inexpensive commercial fertilizers. The large land area suitable for agriculture makes Canada a significant agricultural N r exporter of both grain crops and livestock. Finally, Canada exports petroleum N mainly to the United States. Because of its location and prevailing atmospheric transport patterns, Canada is a net receptor of N r air pollution from the United States, receiving approximately 20% of the N r leaving the U.S. airshed. We found that overall, terrestrial natural ecosystems as well as the atmosphere are in balance between N r inputs and outputs when all N reactive and nonreactive fluxes are included. However, when only reactive forms are considered, almost 50% of N entering the Canadian atmosphere cannot be accounted for and is assumed to be lost to the Atlantic and Arctic oceans or to unmeasured dry deposition. However, agricultural and freshwater landscapes are showing large differences between measured inputs and outputs of N as our data suggest that denitrification in soils and aquatic systems is larger than what models predict. Our work also shows that Canada is a major contributor to the global flow of nitrogen through commercial exports.