Browsing by Subject "Crystalline rock"

Sort by: Order: Results:

Now showing items 1-5 of 5
  • Lehto, Jukka; Puukko, Esa; Lindberg, Antero; Voutilainen, Mikko (2019)
    The distribution coefficient (Kd) of radionuclides on bedrock is one of the key parameters used in the safety analysis of spent nuclear fuel repositories. Typically, distribution coefficients have been determined using crushed rock. However, recent studies have shown that crushing of the rock increases considerably the distribution coefficient compared with the values of intact rock. This study aimed to test if batch sorption experiments using different grain sizes (i.e. mean diameter of grains) can be used to evaluate the Kd of strontium (Sr) and cesium (Cs) on intact crystalline rock, which would decrease the needed experimental time compared with transport experiments. Here we report the results of the batch sorption experiments with crushed rocks and compare the results with those from a recent study performed using electromigration experiments with intact drill core samples (Puukko et al., 2018). The batch sorption experiments were done for rock samples from Olkiluoto, Finland, as a function of grain size and of Cs and Sr concentration. Furthermore, the specific surface areas of the same rock samples with different grain sizes were determined. It was shown that Cs distribution coefficients correlate with specific surface areas of the studied rocks and biotite, the correlation coefficient being 0.95. The Cs distribution coefficient was highest for biotite at about 0.1 m3/kg at 10−4 M cesium concentration and increased systematically to about 1 m3/kg at 10−8 M. Distribution coefficients for rocks were up to about two orders of magnitude lower, being lowest with the rock with the lowest biotite content (3.3%). The distribution coefficient of Sr varied from 0.04 m3/kg to 0.007 m3/kg and behaved in a different manner: it remained constant in two out of three studied rocks in the concentration range of 10−8-10−4 M and only in the case of one rock a decreasing trend was seen at the higher concentration range. It was also shown that batch sorption experiments overestimate the distribution coefficient in respect to intact rock. The decrease of the distribution coefficient as a function of grain size can be estimated using a power law function. It was also shown that estimation of distribution coefficients of Cs and Sr for intact rock by extrapolation of distribution coefficients determined for different grain sizes is not possible without increasing grain size, but in that case diffusion into the grains would also affect the results. A new method was developed for estimating the fraction of the inner surface area of the total surface area of crushed grains. For the mean grain sizes of 0.25 mm and 0.75 mm the fraction of the inner surface was found to be 35–70% and 60–90%, respectively. The inner specific surface area was highest with biotite at 1.2 m2/g and lowest with the rock with lowest biotite content (3.3%) at 0.07 m2/g. The surface area analysis revealed that crushing creates and/or allows access to additional inner surface area that is not measured in intact rock. Furthermore, it was demonstrated that sorption of Cs on crushed rock was dominated by mica minerals in multiple concentrations while the effect of mica minerals on the Kd of Sr was not as straightforward.
  • Voutilainen, Mikko; Miettinen, Arttu; Sardini, Paul; Parkkonen, Joni; Sammaljärvi, Juuso; Gylling, Björn; Selroos, Jan-Olof; Yli-Kaila, Maarit; Koskinen, Lasse; Siitari-Kauppi, Marja (2019)
    The spatial porosity and mineral distribution of geological materials strongly affects transport processes in them. X-ray micro computed tomography (X-mu CT) 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 Aspo, Sweden, and Olkiluoto, Finland, were studied here. The X-mu CT 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-mu CT.
  • Soler, Josep; Meng, Shuo; Moreno, Luis; Neretnieks, Ivars; Liu, Longcheng; Kekalainen, Pekka; Hokr, Milan; Riha, Jakub; Vetesnik, Ales; Reimitz, Dan; Visnak, Jakub; Vopalka, Dusan; Krohn, Klaus-Peter; Tachi, Yukio; Ito, Tsuyoshi; Svensson, Urban; Iraola, Aitor; Trinchero, Paolo; Voutilainen, Mikko; Deissmann, Guido; Bosbach, Dirk; Park, Dong Kyu; Ji, Sung-Hoon; Gvozdik, Libor; Milicky, Martin; Polak, Michal; Gylling, Bjorn; Lanyon, G. William (2022)
    This study shows a comparison and analysis of results from a modelling exercise concerning a field experiment involving the transport and retention of different radionuclide tracers in crystalline rock. This exercise was performed within the Swedish Nuclear Fuel and Waste Management Company (SKB) Task Force on Modelling of Groundwater Flow and Transport of Solutes (Task Force GWFTS). Task 9B of the Task Force GWFTS was the second subtask within Task 9 and focused on the modelling of experimental results from the Long Term Sorption Diffusion Experiment in situ tracer test. The test had been performed at a depth of about 410m in the Aspo Hard Rock Laboratory. Synthetic groundwater containing a cocktail of radionuclide tracers was circulated for 198 days on the natural surface of a fracture and in a narrow slim hole drilled in unaltered rock matrix. Overcoring of the rock after the end of the test allowed for the measurement of tracer distribution profiles in the rock from the fracture surface (A cores) and also from the slim hole (D cores). The measured tracer activities in the rock samples showed long profiles (several cm) for non-or weakly-sorbing tracers (Cl-36, Na-22), but also for many of the more strongly-sorbing radionuclides. The understanding of this unexpected feature was one of the main motivations for this modelling exercise. However, re-evaluation and revision of the data during the course of Task 9B provided evidence that the anomalous long tails at low activities for strongly sorbing tracers were artefacts due to cross-contamination during rock sample preparation. A few data points remained for Cs-137, Ba-133, Ni-63 and Cd-109, but most measurements at long distances from the tracer source (>10mm) were now below the reported detection limits. Ten different modelling teams provided results for this exercise, using different concepts and codes. The tracers that were finally considered were Na-22, Cl-36, Co-57, Ni-63, Ba-133, Cs-137, Cd-109, Ra-226 and Np-237. Three main types of models were used: i) analytical solutions to the transport-retention equations, ii) continuum -porous-medium numerical models, and iii) microstructure-based models accounting for small-scale heterogeneity (i.e. mineral grains, porosities and/or microfracture distributions) and potential centimetre-scale fractures. The modelling by the different teams led to some important conclusions, concerning for instance the presence of a disturbed zone (a few mm in thickness) next to the fracture surface and to the wall of the slim hole and the role of micro-fractures and cm-scale fractures in the transport of weakly sorbing tracers. These conclusions could be reached after the re-evaluation and revision of the experimental data (tracer profiles in the rock) and the analysis of the different sets of model results provided by the different teams.
  • Li, Xiaodong; Puhakka, Eini; Ikonen, Jussi; Söderlund, Mervi; Lindberg, Antero; Holgersson, Stellan; Martin, Andrew; Siitari-Kauppi, Marja (2018)
    The sorption behavior of Se(IV) on Grimsel granodiorite and its main minerals, plagioclase, K-feldspar, quartz and biotite, were investigated in Grimsel groundwater simulant in a large Se concentration range (from 1.66 x 10(-10) M to 1 x 10(-3) M). Experimental results show that the distribution coefficients (K-d values) of Se (IV) on the rock and mineral samples increased with the decreasing of Se(IV) concentration. The sorption of Se (IV) on biotite has the largest K-d value in low concentration area (<10(-7) M) stabilizing between 0.0595 +/- 0.0097 m(3)/Kg and 0.0713 +/- 0.0164 m(3)/Kg. The Kd value of Se(IV) on K-feldspar was the second largest (0.0154 +/- 0.0019 m(3)/Kg in 10(-9) M) while the sorption on quartz was negligible. The sorption behavior of Se(IV) on Grimsel granodiorite followed the same trend as plagioclase, the most abundant mineral in Grimsel granodiorite, with K-d values of 0.0078 +/- 0.0010 m(3)/Kg for Grimsel granodiorite and 0.0085 +/- 0.0016 m(3)/Kg for plagioclase, when Se(IV) concentration was 10(-9) M. HPLC-ICP-MS results show that all the Se(IV) remained in + IV oxidation state after more than 1 month experimental time and speciation modelling proved that the main species in Grimsel groundwater simulant were HSeO3- and SeO32-. Multi-site surface complexation modelling was performed by PHREEQC with the help of molecular modelling techniques which was performed with the CASTEP code implemented into Materials Studio. The modelling results predict that there are three kinds of sorption sites on the surface of biotite mineral, with sorption site densities differing in three magnitudes.
  • Aromaa, Hanna; Voutilainen, Mikko; Ikonen, Jussi; Yli-Kaila, Maarit; Poteri, Antti; Siitari-Kauppi, Marja (2019)
    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.