ARSENIC AND URANIUM TRANSPORT IN SEDIMENTS NEAR ABANDONED URANIUM MINES IN HARDING COUNTY, SOUTH DAKOTA

Sediment samples were analyzed as part of ongoing environmental investigations of historical U mining impacts within Custer National Forest in Harding County, South Dakota. Correlations between As and U content, grain size and soil mineralogy were determined to identify contaminant fate and transport mechanisms. Soil samples collected near the mining source zone and up to 61 km downgradient of the minesites were analyzed. Samples were homogenized and wet sieved through polymer screens, and metal(loid) concentrations were determined using inductively coupled plasma mass spectrometry (ICP-MS). Powder X-ray diffraction (XRD) analysis identified quartz as the primary mineral for all size fractions, with varying amounts of analcime, indicative of volcanic origin. Selected samples were examined for trace mineral composition using scanning electron microscopy (SEM). The presence of Fe sulfides and Fe (hydr)oxides indicate heterogeneity in redox potentials on a microscopic scale. Elevated metal(loid) concentrations were associated with trace concentrations of Fe sulfide, indicating an influence on metal transport during weathering. Sequential chemical extractions (SCE) performed on source sediment fractions demonstrated that most As and U was adsorbed to Fe- and Mn-oxides and carbonates with lesser amounts bound by ion exchange, organics and Fe sulfides. Large changes in U/Th and As/Th ratios were observed to coincide with geochemical changes in the watershed, suggesting that metal(loid)–Th ratios may be used in environmental investigations to identify geochemically-significant watershed conditions. Additionally, temporal sampling results suggest that flooding exerts a profound influence on arsenic bedload concentrations, mostly likely by scouring accumulated Fe and Mn-oxide rinds from aggregate surfaces.