Mechanism of Radionuclide Migration on Saturated and Undisturbed Soil Medium

Abstract

In order to provide technical support and evaluation basis for the development of remediation technology of radioactive contaminated sites and the site selection, design and construction of radioactive waste disposal facilities, the reliable longterm risk assessment for potential nuclear waste repositories and decommissioning of nuclear facilities requires detailed knowledge on the migration behavior of radionuclides in natural, it is necessary to understand the reaction mechanism of radionuclides in the complex geological environment of aquifers. The batch experiments and dynamic undisturbed soil column migration experiments of 90Sr, 137Cs, 238Pu and 241Am were carried out under saturated steadystate flow conditions in fine sand column, a theoretical model of nuclide migration in soil and groundwater environment was constructed, and the irreversible adsorption reaction mechanism of the microinterface was studied through static adsorptiondesorption and dynamic undisturbed soil column migration experiments, and the environmental migration flux of nuclides was calculated. The static adsorption and desorption experiments adopt batch method, and the test medium is fine sand with saturated porous media from an arid mining area in Gansu Province. The fine sand and soil samples according to the solidliquid ratio of 1 g∶9 mL were added into the centrifuge tube, and the nuclide activity concentration was measured after adsorption and desorption equilibriums to obtain the adsorption and desorption isotherms. Dynamic column method used undisturbed soil to ensure the continuity of soil sample medium, original connectivity of void channels and authenticity of stratum. The design and advantages of dynamic column method is to take into account various physical, chemical and biogeochemical reaction processes and complex migration paths of tracers during migration in soil. And the dynamic migration and transformation process of 90Sr, 137Cs, 238Pu and 241Am were studied in saturated porous media with anisotropic timevarying hydrologic characteristics by artificial spraying under controlled laboratory initial conditions and boundary conditions. The results show that the absorption isotherm of 90Sr doesn’t coincide with its desorption isotherm, with an angle at 3238° between them. According to the metastable equilibrium adsorption theory, 90Sr has an irreversible adsorptiondesorption process, and ions exchange is the dominated action for its adsorption. As for 137Cs, 238Pu and 241Am, reversible adsorptiondesorption process are shown, and their adsorptions are mainly attributed to surface complexation. Equilibrium adsorption theory and nonequilibrium adsorption model can be used to describe the migration peak phenomenon of different nuclides in the dynamic soil column experiment, which can be effectively integrated into chemical nonequilibrium and physical nonequilibrium processes. Considering the superposition of convectiondispersion and chemical reaction on solute migration, solute migration equations were established based on the reaction rate equation, and the calculated and measured concentration distribution curves were fitted reasonably to obtain a reaction model that can accurately describe and predict nuclide migration. As for 90Sr, the nonequilibrium adsorption model by transport column was taken into account the firstorder rate coefficient (β) between the dissolved phase and the adsorbed phase. The calculated concentration distribution curve is good agreement with the measured concentration. The fitting results show that the distribution coefficient (Kd) and β of 90Sr in the fine sand aquifer are 085 mL/g and 016 h-1, respectively, in terms of 137Cs, 238Pu and 241Am, the radionuclides concentration distribution curves in equilibrium adsorption and nonequilibrium models are in good agreement with the measured values. Meanwhile the calculated results by two different adsorption models are almost similar, and the Kd are 49×102, 21×104, and 6.0×103 mL/g for 137Cs, 238Pu and 241Am. It shows that the stronger adsorption capacities of the nuclides have the faster rate of the adsorption-desorption in the soil, meanwhile the shorter time for the system reaction equilibrium. At this time, the fitting results of the equilibrium adsorption mode and the nonequilibrium adsorption mode are closer to each other.

Keywords

• radionuclide
• irreversible adsorption
• migration
• non-equilibrium model