Euradwaste '08 - EU Bookshop - Europa
Euradwaste '08 - EU Bookshop - Europa Euradwaste '08 - EU Bookshop - Europa
Figure 1: Schematic of the FEBEX drift with the new boreholes, the packed-intervals, the main fractures and the locations of the Re and I tracers in the FEBEX experiment. Most intervals of new boreholes, closer to the bentonite, showed higher concentration of the main ions than the old radial ones. An increase of Na + and Cl - was observed in all the intervals of FU05.001, particularly relevant in the packed-off section isolating a small lamprophyre dyke (interval 4, Figure 1). Based on the data obtained in these in-situ studies a mass-transfer conceptual model was developed [9, 10]. Additionally, these studied allowed to determine the mean effective diffusion coefficient for Cl - (De = 5.0E-11 m 2 /s). This result will be compared with Cl - diffusion coefficients obtained in the large scale migration experiment that simulates the in-situ FEBEX configuration (bentonite+ large block granite) (WP4.4) [11]. Distribution of the groundwater flow: characterisation and modelling In crystalline rocks water flow takes place in the fractures which are the main conducting paths being advection the dominant transport mechanism. The water flow in the porous rock matrix, with low hydraulic conductivity, is negligible and the main transport mechanism here is diffusion. The predominance of advection over diffusion depends on the characteristics of the fluid flow system. Therefore, the characterisation of the fluid flow system is a key point for evaluating which paths are actually available for RN transport and retention. Fracture network can be very complex and the pore space can be connected or not. It is recognised that small scale features may have an important influence on the overall transport behaviour so that a study of the rock pore space from m to the dm scale was one of the objectives of WP 4.2. At the in-situ scale (dm-m) the characterization of the granite in the FEBEX tunnel was carried out with geophysical experiments, including Natural Gamma, Borehole Ground Penetrating Radar (GPR) and Cross-hole Ultrasonic Tomography. The main objective of the work was to visualize the geometry of the network of fractures in the region between the main boreholes in a quasi 3D-shape. Different fractures cut both FU05.001 and FU05.002 boreholes, all showing low transmissivity (1·10 -11 -1·10 -12 m 2 /s) with exception of the interval 1 of FU05.001 (6-8·10 -10 m 2 /s), at the back of the gallery. The hydro-geological conceptual model of the FEBEX site (10s of meters) was updated on a smaller scale (close to the granite-bentonite interface). Geophysical studies allowed identifying three different fractured regions, slightly parallel to the gallery, and validating indirect visualization methods for the determination of fracture network in a crystalline rock [12]. At a laboratory scale (WP4.2) several techniques were used for the characterisation of the pore structure of different granite samples (Grimsel, Äspö, Olkiluoto, selected cores from the FEBEX site). Different rock matrix characterisation methods (PMMA method, X-ray tomography, confocal laser microscopy) were compared to highlight the applicability and limits of each technique [13]. 330
The links between pore apertures and mineralogy were studied combining PMMA method and autoradiography with electron microscopy (FESEM/EDAX). Heterogeneity, anisotropy and connective pore-network and heterogeneities were identified as a support of transport experiments with solutes and/or colloids (WP 4.3 and WP 4.4). Positron emission tomography (PET) studies were performed to analyse the water flow distribution and colloid transport in a crystalline rock core from Äspö [14]. This non - destructive technique is applied for the direct 3D visualisation of solute transport using PET tracers ( 18 F, 124 I...). The transport paths through the fracture were observed to be modulated by the flow rate and, at localised sites, matrix diffusion was observed [15]. The applicability of PET measurements for investigations of the spatial distribution of transport processes of both dissolved components and colloids in granite was demonstrated. Geometrical description (3D) of the Äspö fractured core was also obtained by X-ray computer micro-tomography (XTC); using this information advanced simulation of the fluid flow can be done. A new experimental approach for non-destructive spatially resolved studies of mapping the mineral composition and the volumetric microstructure of the host rock samples was developed, combining 3D dual-energy cone-beam tomography and X-ray fluorescence [16]. Matrix diffusion. Matrix diffusion (MD) is considered a very important retardation process in crystalline rock above all for not sorbing elements. The state of the art of this process was well described in RETROCK and its theoretical bases in [17]. The effectiveness of matrix diffusion as retardation mechanism depends on the penetration depth into the rock from the water conducting zones, and it is very dependent on the porosity of the rock, the flow rate, RN diffusivity as well as on the flow-wetted surface. To assess its relevance as retention mechanism it is necessary to assess the role of diffusion against advection, if the extension of the RN diffusion within the matrix is limited or not and if the pore system is stable over time. One of the main recognised problems related to diffusion studies is the difficulty of obtaining experimental data partly because of disturbances and artefacts that may exist in laboratory samples. Additionally, diffusion lengths are extremely short (in experimental time span of months - years) above all for highly sorbing radionuclide; thus available data are very scarce. Another process of interest is the diffusion of anions, which can be affected by anionic exclusion, because PA calculations showed that doses are mainly controlled by anionic species 129 I - and 36 Cl - . To demonstrate the role of MD on the retention of these non-sorbing radionuclides is a key point. One of the final goals of RTDC4 studies is to analyse the role of heterogeneities for the matrix diffusion process and to develop models that explicitly take into account the heterogeneity of the rock matrix. In most of the models, matrix diffusion is assumed to be Fickian and homogeneous, but some authors suggested that these assumptions may not be valid [18]; the uncertainties in the migration pathways for contaminants may make inappropriate the deterministic treatment of transport and therefore stochastic methods have been also developed. Indeed, simple models do not include the effect of the heterogeneity in rock properties. First attempts modelling the diffusion in a rock matrix consisting of heterogeneous porosity patterns exist [19, 20, 21]. To validate these models, it is necessary to obtain diffusion coefficients and to correlate diffusion profiles with the physical (and mineralogical) properties of the rock matrix [22]. Thus, a microscale approach to matrix diffusion was started by combining diffusion studies and characterization matrix porosity at a mineral scale [23]. The Rutherford backscattering spectrometry (RBS) is a nuclear ion beam technique that allows measuring concentration profiles in a micrometric scale with a resolution that allows measurements within a single mineral. Apparent diffusion coefficients of uranium could be determined in three different granite types (Grimsel, El-Berrocal and Los Ratones, both from Spain) in different minerals [23]. Differences observed are related to the nature of the mineral grains, particularly grain porosity. The measured Da values for the U diffusion 331
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The links between pore apertures and mineralogy were studied combining PMMA method and<br />
autoradiography with electron microscopy (FESEM/EDAX). Heterogeneity, anisotropy and connective<br />
pore-network and heterogeneities were identified as a support of transport experiments with<br />
solutes and/or colloids (WP 4.3 and WP 4.4).<br />
Positron emission tomography (PET) studies were performed to analyse the water flow distribution<br />
and colloid transport in a crystalline rock core from Äspö [14]. This non - destructive technique is<br />
applied for the direct 3D visualisation of solute transport using PET tracers ( 18 F, 124 I...). The transport<br />
paths through the fracture were observed to be modulated by the flow rate and, at localised<br />
sites, matrix diffusion was observed [15]. The applicability of PET measurements for investigations<br />
of the spatial distribution of transport processes of both dissolved components and colloids in granite<br />
was demonstrated.<br />
Geometrical description (3D) of the Äspö fractured core was also obtained by X-ray computer micro-tomography<br />
(XTC); using this information advanced simulation of the fluid flow can be done.<br />
A new experimental approach for non-destructive spatially resolved studies of mapping the mineral<br />
composition and the volumetric microstructure of the host rock samples was developed, combining<br />
3D dual-energy cone-beam tomography and X-ray fluorescence [16].<br />
Matrix diffusion.<br />
Matrix diffusion (MD) is considered a very important retardation process in crystalline rock above<br />
all for not sorbing elements. The state of the art of this process was well described in RETROCK<br />
and its theoretical bases in [17]. The effectiveness of matrix diffusion as retardation mechanism depends<br />
on the penetration depth into the rock from the water conducting zones, and it is very dependent<br />
on the porosity of the rock, the flow rate, RN diffusivity as well as on the flow-wetted surface.<br />
To assess its relevance as retention mechanism it is necessary to assess the role of diffusion<br />
against advection, if the extension of the RN diffusion within the matrix is limited or not and if the<br />
pore system is stable over time.<br />
One of the main recognised problems related to diffusion studies is the difficulty of obtaining experimental<br />
data partly because of disturbances and artefacts that may exist in laboratory samples.<br />
Additionally, diffusion lengths are extremely short (in experimental time span of months - years)<br />
above all for highly sorbing radionuclide; thus available data are very scarce. Another process of<br />
interest is the diffusion of anions, which can be affected by anionic exclusion, because PA calculations<br />
showed that doses are mainly controlled by anionic species 129 I - and 36 Cl - . To demonstrate the<br />
role of MD on the retention of these non-sorbing radionuclides is a key point.<br />
One of the final goals of RTDC4 studies is to analyse the role of heterogeneities for the matrix diffusion<br />
process and to develop models that explicitly take into account the heterogeneity of the rock<br />
matrix. In most of the models, matrix diffusion is assumed to be Fickian and homogeneous, but<br />
some authors suggested that these assumptions may not be valid [18]; the uncertainties in the migration<br />
pathways for contaminants may make inappropriate the deterministic treatment of transport<br />
and therefore stochastic methods have been also developed. Indeed, simple models do not include<br />
the effect of the heterogeneity in rock properties. First attempts modelling the diffusion in a rock<br />
matrix consisting of heterogeneous porosity patterns exist [19, 20, 21]. To validate these models, it<br />
is necessary to obtain diffusion coefficients and to correlate diffusion profiles with the physical (and<br />
mineralogical) properties of the rock matrix [22].<br />
Thus, a microscale approach to matrix diffusion was started by combining diffusion studies and<br />
characterization matrix porosity at a mineral scale [23]. The Rutherford backscattering spectrometry<br />
(RBS) is a nuclear ion beam technique that allows measuring concentration profiles in a micrometric<br />
scale with a resolution that allows measurements within a single mineral. Apparent diffusion coefficients<br />
of uranium could be determined in three different granite types (Grimsel, El-Berrocal and<br />
Los Ratones, both from Spain) in different minerals [23]. Differences observed are related to the<br />
nature of the mineral grains, particularly grain porosity. The measured Da values for the U diffusion<br />
331