Using chemical models for evaluating the geochemical confinement capacity of a geological barrier - Application to the Centre de Stockage de l'Aube (France)

The feasibility of using a chemical reaction-based approach for evaluating and modelling the role of adsorption reactions in determining the geochemical confinement capacity of natural geological barriers is being studied as part of an on-going R&D programme. The confined superficial aquifer underlying the Centre de Stockage de l'Aube facility, a geological barrier for this site, has been used as a case study with the following aims. First, development of a site characterisation protocol and demonstration of its use to determine the principal geochemical characteristics of aquifer materials using batch experiments and to represent the information obtained in terms of a chemical model. The experimental results obtained for Ni2+ partitioning as a function of total Ni, pH, total Ca and total solid can be satisfactorily represented in terms of reactions with an ion exchange site and a single amphoteric surface hydroxyl site with ferrihydrite reaction constants. A second objective is the incorporation of the reactions in a coupled geochemistry/transport code, and to verify the applicability of the coupled code predictions for Ni2+ mass transfer by comparison with the results obtained during column tracer experiments. The breakthrough curve and equilibrium solid phase Ni loading, predicted by a one-dimensional coupled model for a column tracer experiment, agree closely with observed data. Additional studies are underway to reduce model conditionality, to extend the adsorption model to other analogue cations and anions, to incorporate the effect of natural organic matter and to take into consideration precipitation/dissolution of amorphous Fe surface phases. (C) 1997 Elsevier Science B.V.