RESUMO
Numerical simulation of cation exchange and mineral precipitation/dissolution reactions using the multiphase reactive geochemical transport code TOUGHREACT has provided important insight into the distribution of (90)Sr among layers of geologic strata in a complex vadose zone at the U. S. Department of Energy's Idaho National Laboratory. During a transfer operation in November 1972, 70.4 m(3) of acidic, high ionic strength liquid containing 15,900 Ci of (90)Sr was released over five days into alluvial gravels 137 m above the Snake River Plain Aquifer. Sampling data from perched water zones 33 m below the release contain very high levels of (90)Sr as do soil samples obtained nearer the point of release. Use of traditional simulation approaches using laboratory-measured constant partitioning coefficients (K(d)) cannot simultaneously explain perched water and soil concentrations. To address the discrepancy, a reactive transport approach was adopted to include competitive cation exchange, dissolution/precipitation of calcite, carbon dioxide gas production and transport, and gibbsite precipitation. Simulation results using this model suggest that some of the (90)Sr could have been transported very rapidly immediately after the release with the acceleration facilitated by competition for cation exchange sites with high sodium concentrations in the released liquid and calcium dissolved from calcite, and to a lesser extent by formation of aqueous complexes with nitrate. Once the leading edge of the liquid assemblage was flushed from the alluvium, the mobility of the remaining (90)Sr decreased significantly in the absence of the competing cations. Calculations indicate that there should be a net increase in calcite, suggesting that (90)Sr could be entrained in the mineral lattice, but insufficient field data exist for confirmation. Sensitivity studies show that the cation exchange selectivity coefficients were the most sensitive individual parameters determining the (90)Sr distribution. However, the most sensitive overall quantity was the total ion exchange capacity which is a function of the moles of exchange sites per volume of pore water, the cation exchange capacity, and the total volume wetted by the infiltrating solution. In contrast, the future mobility of (90)Sr was found to be relatively insensitive to the normal range in the composition of influxing precipitation and anthropogenic waters.
