Mass-Balance Modeling of Metal Loading Rates in the Great Lakes

Major elements and nutrients are key water quality monitoring targets in the Great Lakes, but large-scale and long-term data for (trace) metals remains comparatively scarce. Consequently, the sources and processes controlling metal loading rates and potential accumulation in the lakes are not as well constrained. Here, we present a comprehensive assessment of select metal loads in the Great Lakes basin, aggregating tributary and connecting channel loads as well as estimates for atmospheric input and sedimentation. In total, 26,845 hydrometric and water quality datapoints from major environmental surveillance programs were compiled into mass-balance calculations and dynamic simulations for 1980-2020. Conservative element (Na, Cl) loads were used to calibrate the black-box approach, and mass-balance for these elements could be achieved at ≥90% and long-term trends accurately reproduced. In contrast, biogeochemically reactive (trace) metals Cu, Ni, Zn and Pb displayed highly variable source-sink behavior across the Great Lakes. Our results show that i) atmospheric inputs, tributary loads, and sedimentation all affect the concentrations and temporal trends of the studied metals but differently in the upper versus lower lakes, ii) smaller tributaries can be disproportionately important to lake-wide metal budgets, and iii) current loading rates may yield increasing lake-wide average Cl concentrations (e.g., up to 2.3 mg/L in Lake Superior) but decreasing metal concentrations (e.g., down to <0.25 μg/L Cu in Lake Ontario) by 2100. This work provides important quantitative baselines for metal loads in the Great Lakes and may help optimize surveillance and management strategies for the preservation of Great Lakes water quality.