Kinetics of the adsorption and desorption of radionuclides of Co, Mn, Cs, Fe, Ag and Cd in freshwater systems: experimental and modelling approaches

The sorption and release kinetics of Mn-54, Co-58, Fe-59, Cd-109, Ag-110m and Cs-134 by freshwater suspended particles were investigated to better identify the biogeochemical processes involved and to obtain suitable data for improving models describing radionuclide migration in freshwater streams. In order to observe any seasonal variability in the interaction of radionuclides with natural particles, experiments were performed both in winter and in summer during a phytoplanktonic bloom. Two kinetic models are compared in this paper: the one-step reversible model, based on the hypothesis that the transfer of radionuclides between water and suspended solids is governed by a reversible reaction, and the two-successive-step reversible model, which assumes two distinct types of sites or reactions on the solid phase. The one-step reversible model is generally unable to describe properly the exchange kinetics; this result shows that at least two processes are generally involved in radionuclide exchange between water and suspended particles. On the contrary, a model involving the existence of two successive reversible reactions properly simulates both the sorption and release kinetics. The determination of the kinetic coefficients allows quantitative assessment of the relative importance and kinetics of the processes. In particular, it has been shown that, except for Cs and Cd, major fractions of the radionuclides are associated at equilibrium with particulate sites involving strong interactions. The kinetics to reach this equilibrium depend on seasonal conditions, especially for Co and Mn: the transfer of Co and Mn to particulate sites involving strong interactions is much slower in winter. The distribution of the radionuclides between water and particulate sites involving weak interactions also shows seasonal variations for Co, Mn, Fe and Ag: the capacity to associate radionuclides is much higher in summer for Co and Mn, while the inverse tendency is observed for Fe and Ag. For Cs and Cd, no significant seasonal differences were observed. (C) 2001 Elsevier Science Ltd. All rights reserved.