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The Finnish plan for the final deposition of nuclear waste is deposition deep in the crystalline bedrock. In the safety case of the final deposition, matrix diffusion, along with sorption, is considered the most important retarding factor for radionuclide transport in the geosphere. We set out to measure matrix diffusion in the gas phase for two 80 cm long drill-core samples from Olkiluoto, Finland. One sample consisted of veined gneiss and the other of pegmatitic granite. The measurements were taken in the laboratory with an advection-diffusion measurement setup that uses nitrogen as the carrier gas and helium as the tracer. The measured breakthrough curve for the veined gneiss sample could be interpreted with a homogeneous mathematical model, and the result for the effective diffusion coefficient ( $$D_{\mathrm{e}}$$ ), $$4.2 \pm 0.9 \times 10^{-10}\,\frac{\mathrm {m}^2}{\mathrm {s}}$$ , agreed with previous results for veined gneiss from through-diffusion experiments in the gas phase. The breakthrough curve for the pegmatitic granite sample required a three-component model because of high variations in the local transport parameters (porosity, diffusion coefficient). The spatial distributions of porosities were characterized with the $$^{14}$$ C-polymethylmethacrylate-autoradiography technique. The result, $$D_{\mathrm{e}} = \left( 32 \pm 7\right) \times 10^{-10}\,\frac{\mathrm {m}^2}{\mathrm {s}}$$ , for the most abundant component was also in accordance with the previous through-diffusion results. Comparison of the two measurements showed that diffusion phenomena can be very sensitive to the microstructure of rock even when macroscopic properties such as porosity remain the same. The retarding effect of matrix diffusion from flow was clearly observed for both samples, and knowledge of the sample structure, rock types, and mineralogy were concluded to be vital in analyzing and interpreting the results. [ABSTRACT FROM AUTHOR]

Abstract: 3D distributions of minerals and porosities were determined for rock-core samples that included water-conducting fractures. The analysis of these samples was performed using conventional petrography methods, C-14-PMMA porosity analysis and X-ray tomography. It seems that the properties of rock around a water-conducting fracture depend on so many uncorrelated factors that no clear pattern emerged even for rock samples with a given type of fracture. We can conclude, however, that the present combination of methods can be used to infer novel structural information about alteration zones adjacent to fracture surfaces. [Copyright &y& Elsevier]

• Similar transport experiments were performed in laboratory and in situ conditions. • Analytical solution was derived to model the measured breakthrough curves. • Transport of HTO and 36 Cl is retarded more in laboratory than in situ conditions. • Anion exclusion reduces the retention parameters of 36 Cl compared with HTO. • In-situ distribution coefficient of 22 Na is ten times smaller than previous laboratory studies indicate. In some countries the spent nuclear fuel produced by nuclear power plants will be deposited in crystalline granitic rock formations. In Finland, a repository for the spent nuclear fuel is being built at Olkiluoto. The safety assessment of the repository requires a careful determination of the transport properties of the bedrock.The porosity of the bedrock and the effective diffusion coefficients and distribution coefficients of different radionuclides for the bedrock are used as the main parameters in the safety assessment calculations. It has been questioned whether the parameters determined using laboratory experiments can be used to estimate the parameters in the in situ conditions.In this study, laboratory and in situ water phase diffusion experiments (WPDEs) were performed to resolve the issue.In the experiments, the transport of tritiated water (HTO), 36 Cl , and 22 Na was studied using similar experimental setups. Mathematical models were constructed and solved to determine the transport parameters from the measured breakthrough curves. On average, the in situ WPDEs resulted in 20 (± 6)% smaller porosities and 32 (± 10)% smaller effective diffusion coefficients for HTO and 36 Cl than the laboratory WPDEs. It was also found that in veined gneiss, the most dominant rock type of the Olkiluoto bedrock, anion exclusion reduced the retention parameters of 36 Cl compared with those of HTO. Furthermore, the distribution coefficient of 22 Na for veined gneiss was about one order of magnitude smaller in the in situ conditions than in previous laboratory batch sorption experiments. The effects of the results on the safety assessment were evaluated and discussed. [ABSTRACT FROM AUTHOR]

Abstract 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. Highlights • 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. [ABSTRACT FROM AUTHOR]

Abstract The spatial porosity and mineral distribution of geological materials strongly affects transport processes in them. X-ray micro computed tomography (X-μCT) has proven to be a powerful tool for characterizing the spatial mineral distribution of geological samples in 3-D. However, limitations in resolution prevent an accurate characterization of pore space especially for tight crystalline rock samples and 2-D methods such as C-14-polymethylmethacrylate (C-14-PMMA) autoradiography and scanning electron microscopy (SEM) are needed. The spatial porosity and mineral distributions of tight crystalline rock samples from Äspö, Sweden, and Olkiluoto, Finland, were studied here. The X-μCT were used to characterize the spatial distribution of the main minerals in 3-D. Total porosities, fracture porosities, fracture densities and porosity distributions of the samples were determined using the C-14-PMMA autoradiography and characterization of mineral-specific porosities were assisted using chemical staining of rock surfaces. SEM and energy dispersive X-ray spectroscopy (EDS) were used to determine pore apertures and identify the minerals. It was shown that combination of the different imaging techniques creates a powerful tool for the structural characterization of crystalline rock samples. The combination of the results from different methods allowed the construction of spatial porosity, mineral and mineral grain distributions of the samples in 3-D. These spatial distributions enable reactive transport modeling using a more realistic representation of the heterogeneous structure of samples. Furthermore, the realism of the spatial distributions were increased by determinig the densities and porosities of fractures and by the virtual construction heterogeneous mineral distributions of minerals that cannot be separated by X-μCT. [ABSTRACT FROM AUTHOR]

The sorption of Ra on Olkiluoto biotite in the context of deep geological disposal of spent nuclear fuel was studied with isotherm batch sorption experiments. Ba was used as an analog for Ra in the experiments and modeling studies. A wide concentration range of Ra/Ba was used in the isotherm studies (2.6 × 10−9 M to 1 × 10−3 M) in addition to four different Olkiluoto reference groundwaters with salinity types ranging from fresh to saline. Experimental results show that both in the fresh and saline reference groundwaters, the distribution coefficients of Ra tend to decrease in the higher isotherm concentrations of Ba. With one reference groundwater, the distribution coefficients increased with the concentration of Ba due to significant coprecipitation of Ra. With the fresh reference groundwaters, the distribution coefficients of Ra were consistently approximately one order of magnitude lower than in the saline reference groundwater. A PHREEQC multi-site complexation model coupled with an optimization tool in Python was used to interpret the experimental Ra sorption results. Molecular modeling with CASTEP code implemented into Materials Studio was used to update the PHREEQC model with more realistic biotite sorption site density data. It was observed that while the multi-site model predicts the sorption of Ra well in lower isotherm concentrations, auxiliary reactions of Ra disrupt the model in high Ba isotherm concentrations. The experimental and modeled distribution coefficient data of Ra on biotite can be used in the safety case calculations of the deep geological disposal of spent nuclear fuel in Finland and Sweden. • Data on the sorption of radium can be used for safety case in nuclear waste disposal. • Sorption of radium varies depending on the chemistry of surrounding groundwater. • Radium is a weak competitor in sorption reactions against smaller cations. • Radium's sorption magnitude and mechanisms can be accurately modeled. [ABSTRACT FROM AUTHOR]