The role of natural organic matter in the migration behaviour of americium in the Boom clay - Part II: analysis of migration experiments

Full text of publication follows: In demonstrating the suitability of Boom Clay as a potential site for the disposal of radioactive waste in Belgium, the role of the relatively high amount of Natural Organic Matter (NOM) present in the Boom Clay on the mobility of critical radionuclides needs investigation. Trivalent actinides and lanthanides form strong complexes with humic substances. Complexation of these trivalent radionuclides with NOM present in the Boom Clay may have opposing effects. If complexed by the aqueous phase (mobile) NOM, radionuclide transport will be governed by the mobility of these dissolved radionuclide-NOM species. If complexed by the solid phase (immobile) NOM, migration will be retarded. One of the aims of the EC projects TRANCOM-Clay and TRANCOM-II was to investigate the role of mobile NOM as radionuclide carrier with the objective of deriving conceptual models that can be implemented in repository performance assessment (PA) models. A separate paper describes the results of column migration experiments involving the transport of 241Am-14C-NOM complexes through Boom Clay cores. This paper describes the transport model, POPCORN, that was developed to describe and evaluate the influence of NOM on radionuclide transport in clay, taking into account attachment/detachment rates of NOM to clay surfaces and the kinetics of RN complexation to, and destabilization from, NOM. The POPCORN model was used to evaluate diffusion experiments involving injection of 14C-labelled NOM in Boom Clay cores. Model fits were obtained by varying the rates of filtration of NOM by attachment to the surface of the clay matrix. POPCORN was then used to analyse the 241Am-14C-NOM migration experiments. The stability properties of the 241Am-NOM were characterised by kinetic constants, and good matches to the migration data were achieved for the experiments. The findings suggest that a small sub-population of the original 241Am-OM is the most stable, and that this sub-population has specific transport characteristics, including low dispersivity and a potential for filtering. Such characteristics may be representative of larger, more stable, but less mobile 241Am-OM complexes. In summary, the key processes governing 241Am migration are the rate of 241Am-OM destabilization and the rates of attachment and detachment of OM on the clay surfaces. Correlations between different transport parameters have been identified, and these findings offer means of extrapolating parameter values for application of the model to larger-scale problems. (authors)