The diffusion of radionuclides is an important safety aspect for nuclear waste disposal in argillaceous host rocks. A long-term diffusion experiment, termed DI-A, is being carried out at the Mont Terri Rock Laboratory in the Opalinus Clay formation. The aim of this experiment is the understanding of the migration and sorption behaviour of cationic and anionic species in consolidated clays. This study reports on the experimental layout and the first results obtained from the DI-A experiment, which include the investigation of HTO, 22Na+, Cs+, and I- migration during a period of 1 year by analysing these tracers in the water circulating in the borehole. In addition, results obtained from through-diffusion experiments on small-sized samples with HTO, I-, and 36Cl- are presented. The decrease of tracer concentrations in the borehole is fastest for Cs+, followed by 22Na+, HTO, and finally I-. The chemical composition of the artificial pore water in the borehole shows very little variation with time, thus indicating almost no chemical disturbance around the borehole. Through-diffusion experiments in the laboratory that were performed parallel to the bedding plane with two different methods yielded effective diffusion coefficients for HTO of 4-5×10-11 m2 s-1 and significantly lower ones for anions Cl- and I- (0.7-1.6×10-11m2s-1). The results indicate the importance of anion exclusion effects arising from the negatively charged clay surfaces. Furthermore, they demonstrate the anisotropic diffusion properties of the clay formation with significantly increased diffusion rates parallel to bedding relative to the perpendicular direction. The tracer data of the in situ experiment were successfully described with 2D diffusion models using diffusion and sorption parameters obtained from the above mentioned and other laboratory studies. The modelling results indicate that HTO and I- diffused with no retardation. The retardation of Na+ and Cs+ could be described by empirical sorption expressions from previously derived batch sorption (Cs+) or diffusion (Na+) experiments.Overall, the obtained results demonstrate the feasibility of the technical concept to study the diffusion of non-sorbing and sorbing tracers in consolidated clays.
a NAGRA, Hardstrasse 73, Wettingen CH-5430, Switzerland
b PSI, Villigen CH-5232, Switzerland
c CSIC-IJA, Barcelona E-08028, Spain
d CIEMAT, Madrid E-28040, Spain
e ENRESA, Madrid E-28043, Spain
f IRSN, F-Fontenay-aux-Roses 92265, France