The controls on the mobility and fate of arsenic in lakes impacted by historical gold ore roasting in northern Canada have been examined. A detailed characterization of arsenic solid and aqueous phases in lake waters, lake sediments and sediment porewaters as well as surrounding soils was conducted in three small lakes (<200ha) downwind and within 5 km of the historic mining and roasting operations of Giant Mine (Northwest Territories). These lakes are marked by differing limnological characteristics such as area, depth and organic content. Radiometric age-dating shows that the occurrence of arsenic trioxide in lake sediments coincides with the regional onset of roasting activities. Quantification by advanced electron microscopy shows that arsenic trioxide accounts for up to 6 wt% of the total arsenic in sediments. The bulk (>80 wt%) of arsenic is contained in the form of secondary sulphide precipitates, with iron oxy-hydroxides hosting a minimal amount of arsenic (<1 wt%). Soluble arsenic trioxide particles act as the primary source of arsenic into sediment porewaters. Dissolved arsenic in reducing porewaters both precipitates in-situ as secondary sulphides, and diffuses upwards into the overlying lake waters. Geogenic arsenic phases are present in sediments in low concentrations and are not considered a significant source of arsenic to porewaters or lake waters. Sediment-water interface diffusive flux calculations suggest that the diffusion of dissolved arsenic from porewaters, combined with lake water residence time, are the predominant mechanisms controlling arsenic concentrations in lake waters.
Keywords: Arsenic mobility; Arsenic speciation; Arsenic trioxide; Giant mine; Subarctic palaeolimnology.
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