Column Experiments for Radionuclide Adsorption Studies of the Culebra Dolomite: Retardation Parameter Estimation for Non-Eluted Actinide Species

Abstract

The U.S. Department of Energy (DOE) has been developing a nuclear waste disposal facility, the Waste Isolation Pilot Plant (WIPP), located approximately 42 km east of Carlsbad, New Mexico. The WIPP is designed to demonstrate the safe disposal of transuranic wastes produced by the defense nuclear-weapons program. Performance assessment analyses (U.S. DOE, 1996) indicate that human intrusion by inadvertent and intermittent drilling for resources provide the only credible mechanisms for significant releases of radionuclides horn the disposal system. These releases may occur by five mechanisms: (1) cuttings, (2) cavings, (3) spallings, (4) direct brine releases, and (5) long-term brine releases. The first four mechanisms could result in immediate release of contaminant to the accessible environment. For the last mechanism, migration pathways through the permeable layers of rock above the Salado are important, and major emphasis is placed on the Culebra Member of the Rustler Formation because this is the most transmissive geologic layer in the disposal system. For reasons of initial quantity, half-life, and specific radioactivity, certain isotopes of Th, U, Am, and Pu would dominate calculated releases from the WIPP. In order to help quanti~ parameters for the calculated releases, radionuclide transport experiments have been carried out using five intact-core columns obtained from the Culebra dolomite member of the Rustler Formation within the Waste Isolation Pilot Plant (WIPP) site in southeastern New Mexico. This report deals primarily with results of mathematical analyses related to the retardation of %J%, 24%, and 24'Am in two of these cores (B-Core - VPX26-11A and C-Core - VPX28-6C). All B-Core transport experiments were done using Culebra-simukmt brine relevant to the core recovery location (the WIPP air-intake shaft - AIS). Most experiments with C-Core were done with AIS brine with some admixture of a brine composition (ERDA-6) that simulated deeper formation brines. No significant changes in transport behavior were observed for changes in brine. Hydraulic characteristics (i.e., apparent porosity and apparent dispersion coefficient) for the cores were obtained via experiments using conservative tracer `Na. Elution experiments carried out over periods of a few days with tracers `*U and %Np indicated that these tracers were weakly retarded as indicated by delayed elution of these species. Elution experiments with tracers `%, 24'Pu, and 24'Ani were performed, but no elution of any of these species was observed in any flow experiment to date, including experiments of up to two years duration. However, B-Core was subjected to tomographic analysis from which a retardation factor can be inferred for%. Moreover, the fact of non- elution for 24*Pu and 24'Am after more than two years brine flow through C-Core can be coupled with the minimum detectable activity for each of these species to compute minimum retardation factors in C-Core. The retardation factors for all three species can then be coupled with the apparent hydraulic characteristics to estimate an apparent minimum solutionhock distribution coefficient, &, for each actinide. The specific radionuclide isotopes used in these experiments were chosen to facilitate analysis. Even though these isotopes are not necessarily the same as those that are most important to WIPP performance, they are isotopes of the same elements, and . their chemical and transport properties are therefore identical to those of isotopes in the WIPP inventory. The retardation factors and & values deduced from experimental results strongly support the contention that sorption in the Culebra provides an effective barrier to release of Th, Pu, and Am during the regulatory period.