Experimental measurements and integrated modelling studies of actinide sorption onto cement

An Integrated Cement Sorption Model (ICSM) for actinides onto Ordinary Portland Cement (OPC) is developed. The experimental measurements using the batch sorption technique for actinides onto cement and constituent minerals, which were considered in the modelling calculations, are also described. The actinide elements studied (thorium, uranium, neptunium, plutonium and americium) were strongly sorbed onto OPC. An initial comparison of the experimental data relating the sorption values of actinides onto cement-component phases with those onto OPC is carried out. The results suggest that the Calcium Silicate Hydrate (C-S-H) phases were found to be the most likely candidates to be the dominant-sorbing phases in order to describe the sorption of a actinides onto OPC. An approach to develop the integrated cement sorption model, based on a thermodynamic surface complexation model, is described with discussions on the possible mineralogy and phase distribution of OPC. Another approach than sorption, assuming that co-precipitation on the surface of the cement phase dominates 'sorption', is proposed and discussed. A scoring system is introduced to assess the applicability of the proposed ICSMs. It is suggested that the thermodynamic sorption model is recommended for the sorption of ionic species and the surface co-precipitation model is recommended for the sorption of neutral species though the sorption model is still recommended to be used to model OPC-based systems. (author)