PNNL

Abstract

The phase distribution of trace metals and oxyanions was investigated within a South Texas watershed hosting a high density of surface uranium mine pits and tailings. The objectives of the study were to evaluate the potential impact of these old uranium mining sites on the watershed with particular emphasis on spatial and temporal changes in water quality of a reservoir that serves as the major source of freshwater to a population of ~350,000 people in the region. A livestock pond, bordered by uranium mine tailings, was used as a model case-study site to evaluate the cycling of uranium mine-derived oxyanions under changing redox conditions. Although the pond showed seasonal thermal and chemical stratification, geochemical cycling of metals was limited to Co and Pb, which seemed to be mostly associated with redox cycling of Mn mineral phases, and U, which suggested reductive precipitation in the pond’s hypolimnion. Uranium levels, however, were too low to support strong inputs from the tailings into the water column of the pond. The strong relations observed between particulate Cr, Cs, V and Fe suggest that these metals are associated with a stable particulate phase (probably allochthonous aluminosilicates) enriched in unreactive iron. This observation is supported by a parallel relationship in sediments collected across a broad range of sediment depositional processed (and histories) in the basin. Arsenic, though selectively enriched in the pond’s water column, remained stable and mostly in solution throughout the depth of the profile and showed no sign of geochemical cycling or interaction with Fe-rich particles. We found no evidence of anthropogenic impacts of U mines beyond the purely local scale. Arsenic does decrease in concentration downstream of uranium mining sites but its presence within the Nueces drainage basin is related to interactions between surface and ground waters with uranium-rich geological formations rather than long-scale transport of contaminants downstream of the U mine pits and tailings. As in Lyssy pond, arsenic (and other oxyanions) in Lake Corpus Christi’s water column are not affected by the abundant presence of Fe-rich particles but instead behave conservatively throughout the entire period of study. A quantitative mass balance model, constructed using monthly hydrological data for the reservoir, provides quantitative evidence of seasonal evaporative concentration of as in surface waters demonstrating the predominance of hydrodynamic constraints, over geochemical ones, on the cycling of this metal in selected aquatic systems.