Natural attenuation reactions at a uranium mill tailings site, western U.S.A

This paper presents a modeling analysis of the geochemical evolution of a contaminated sandy aquifer at a uranium mill tailings site in the western United States. The tailings pond contains fluids having a pH of 1.5 to 3.5 and high levels of As, Be, Cd, Cr, Pb, Mo, Ni, Se, 226Ra, 228Ra, 230Th, 238U, and 234U. Seepage of tailings fluids into the aquifer has formed a low-pH ground water plume. The reclamation plan is to install a low-permeability cover on the tailings pond to stop the seepage and allow the plume to be attenuated by reactions with the aquifer matrix and flushed by uncontaminated upgradient ground water. To evaluate this reclamation scenario, ground water and sediment core samples were analyzed along one flowpath. Speciation-solubility and mass-transfer modeling revealed two sets of chemical reactions for acid seepage and flushing, respectively. The current concentrations and distribution of ground water constituents can be interpreted as being controlled by stepwise pH-buffer reactions with calcite, amorphous aluminum hydroxide, and amorphous iron hydroxides. These buffer reactions divide the aquifer into zones of near-constant pH, separated by interface zones. For the flushing stage, it is predicted that reactions with surface-bound species will dominate the reaction paths, and more pore volumes are required to neutralize the plume than predicted by models that do not consider surface reactions. Direct mineralogical and surface analysis is needed to substantiate this assertion.