Experimental and modeling study of adsorption–desorption processes with application to a deep-well injection radioactive waste disposal site

Radionuclide (Sr-90 and Cs-137) behavior in the subsurface environment was evaluated with respect to natural attenuation, sorption and desorption kinetics, and equilibrium. Batch experiments were conducted with synthesized groundwater or acid (NaNO3; pH ≈3) solutions under different temperature (T=20 and 70 °C) and pressure (P=Patm and P=3 MPa) conditions. Samples of sedimentary rock were selected as the solid phase from a radioactively contaminated site associated with deep-well injection of the radioactive waste. Groundwater and a NaNO3 waste–brine solution were used as the liquid phase. All experiments revealed hysteresis in radionuclide adsorption. Moreover, some of the experiments indicated that the adsorption process may be irreversible. A simultaneous temperature and pressure increase leads to anomalous behavior of the adsorption kinetics: a period of a rapid concentration drop of the radionuclides in solution, which is caused by their sorption uptake, is changed by a stage of a gradual increase in the corresponding concentrations. To explain the observed phenomena, several hypotheses were examined. Thus, an analytical model describing the mutual interference of adsorption kinetics and dissolution of carbonate minerals was developed resulting in a nonmonotonic behavior of the concentration curves obtained at the adsorption stage. For the description of the batch experiments with radionuclides at room temperature and atmospheric pressure, a dual-site adsorption model has been used.