Through diffusion experiments to study the diffusion and sorption of HTO, 36Cl, 133Ba and 134Cs in crystalline rock

The spent nuclear fuel in Finland will be deposited in crystalline granitic rock in Olkiluoto, Finland. As a part of the safety assessment of the repository, series of extensive in-situ sorption and diffusion experiments and supplementary laboratory work has been done in the Olkiluoto site. Through Diffusion Experiment in a laboratory (TDElab) aims to provide applicable data for the ongoing in-situ experiment in Olkiluoto. This laboratory scale experiment resembles the in-situ experiment and aims to gain information on possible effects in values of distribution coefficients, effective diffusion coefficient and porosity that are caused by differences in laboratory and in-situ conditions. The through diffusion and sorption of tracer solution with known activities of HTO, 36Cl, 133Ba and 134Cs were studied in a decimeter scale sample of veined gneiss, which is one of the main rock types in Olkiluoto. The measured breakthrough curves were modeled taking into account the porosity of the rock and diffusion and sorption of the radionuclides using Time-Domain Random Walk (TDRW) simulations. The porosities of 0.7–0.8% were determined for the rock and effective diffusion coefficients of (3.5 ± 1.0) × 10−13 m2/s and (3.0 ± 1.0) × 10−13 m2/s were determined for HTO and 36Cl, respectively. The porosity and effective diffusion coefficients were found to be in agreement with previous results for veined gneiss. Furthermore, distribution coefficients of (1.0 ± 0.3) × 10−4 m3/kg and (2.0 ± 0.5) × 10−3 m3/kg were determined for 133Ba and 134Cs, respectively, using information about the effective diffusion coefficient determined for HTO. The distribution coefficients were found to be significantly smaller than the ones determined for crushed rock in previous studies and slightly smaller than the ones from previous in-diffusion experiments. •The distribution and effective diffusion coefficients of intact rock were determined using through diffusion experiments.•TDRW simulations are capable of reproducing the measured breakthrough curves.•The distribution coefficients for intact rock were significantly smaller than previous results for crushed rock.•Later the results can be compared with results from similar in-situ experiment.•The results can be used for the safety assessment of nuclear waste repositories.