Geochemical and hydrodynamic controls on arsenic and trace metal cycling in a seasonally stratified US sub-tropical reservoir

摘要

The phase distribution of trace metals and oxyanions, including U and As, in 2 surface water bodies was investigated within a South Texas watershed hosting a high density of surface U mine pits and tailings. The objectives of the study were to evaluate the environmental legacy of U mining, with particular emphasis on the spatial and temporal variability of water quality in Lake Corpus Christi, a downstream reservoir that serves as the major water resource to a population of similar to350,000 people in the region. Lyssy Pond, a livestock pond bordered by U mine tailings, was used as a model case-study site to evaluate the cycling of U 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 was correlated 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 relationships observed between particulate Cr, Cs, V, and Fe suggest that these metals are associated with a stable particulate phase (probably allochthonous alumino-silicates) enriched in unreactive Fe. This observation is supported by a parallel relationship in sediments collected across a broad range of sediment depositional processes (and histories) in the basin. Arsenic, though selectively enriched in the pond's water column, was dominated by dissolved species throughout the depth of the profile and showed no sign of geochemical cycling or interaction with Fe-rich particles. Arsenic (and other oxyanions) in the water columns of Lake Corpus Christi and Lyssy pond were not affected by the abundant presence of Fe-rich particles but instead behaved conservatively. No evidence was found of anthropogenic impacts of U mines beyond the purely local scale. Arsenic's presence within the Nueces drainage basin is related to interactions between surface and groundwaters with U- and As-rich geological formations rather than large-scale transport of contaminants downstream of the U mine pits and tailings. 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 over geochemical constraints, on the cycling of this element. (C) 2004 Elsevier Ltd. All rights reserved.