Modelling transport of reactive tracers in a heterogeneous crystalline rock matrix.

A numerical reactive transport model for crystalline rocks is developed and evaluated. The model is based on mineral maps generated by X-ray micro computed tomography (X-µCT); the maps used have a resolution of approximately 30 µm and the rock samples are on the cm scale. A computational grid for the intergranular space is generated and a micro-DFN (Discrete Fracture Network) model governs the grid properties. A particle tracking method (Time Domain Random Walk) is used for transport simulations. The basic concept of the model can now be formulated as follows; "when a particle is close to a reactive mineral surface it has a certain probability to get sorbed during a certain time span. Once sorbed it will remain so a certain time". The model requires a number of input parameters that represent the sorption properties of the reactive minerals. Attempts are made to relate the parameters to traditional distribution parameters. The model is evaluated by comparisons with recent laboratory experimental data. These experiments consider two rock types (veined gneiss and pegmatitic granite) and two radionuclides (cesium and barium). It is concluded that the new reactive transport model can simulate the experimental data in a consistent and realistic way.

Transport of oxygen into granitic rocks: Role of physical and mineralogical heterogeneity.

The rock matrix of granites is expected to be an important buffer against the dispersion of contaminants, e.g. radionuclides, and against the ingress of oxygenated glacial meltwater. The influence of matrix heterogeneity on O2 diffusive transport is assessed here by means of numerical experiments based on a micro-Discrete Fracture Network (micro-DFN) representation of the diffusion-available pore space along with random realisations of idealized biotite grains, to simulate the heterogeneous nature of granitic rocks. A homogeneous-based analytical solution is also presented and used to assess possible deviations of the numerical experiments from the assumption of homogeneity. The analytical solution is also used to test upscaled values of mineral surface area. The numerical experiments show that the matrix behaves as a composite system, with the coexistence of fast and slow diffusive pathways. This behavior is more evident at low Damköhler numbers. Our interpretation of the numerical experiments points out the importance to properly characterise the heterogeneity of the rock matrix.

Microtomography-based Inter-Granular Network for the simulation of radionuclide diffusion and sorption in a granitic rock.

Field investigation studies, conducted in the context of safety analyses of deep geological repositories for nuclear waste, have pointed out that in fractured crystalline rocks sorbing radionuclides can diffuse surprisingly long distances deep into the intact rock matrix; i.e. much longer distances than those predicted by reactive transport models based on a homogeneous description of the properties of the rock matrix. Here, we focus on cesium diffusion and use detailed micro characterisation data, based on micro computed tomography, along with a grain-scale Inter-Granular Network model, to offer a plausible explanation for the anomalously long cesium penetration profiles observed in these in-situ experiments. The sparse distribution of chemically reactive grains (i.e. grains belonging to sorbing mineral phases) is shown to have a strong control on the diffusive patterns of sorbing radionuclides. The computed penetration profiles of cesium agree well with an analytical model based on two parallel diffusive pathways. This agreement, along with visual inspection of the spatial distribution of cesium concentration, indicates that for sorbing radionuclides the medium indeed behaves as a composite system, with most of the mass being retained close to the injection boundary and a non-negligible part diffusing faster along preferential diffusive pathways.

Continuum-based DFN-consistent numerical framework for the simulation of oxygen infiltration into fractured crystalline rocks.

We present an enhanced continuum-based approach for the modelling of groundwater flow coupled with reactive transport in crystalline fractured rocks. In the proposed formulation, flow, transport and geochemical parameters are represented onto a numerical grid using Discrete Fracture Network (DFN) derived parameters. The geochemical reactions are further constrained by field observations of mineral distribution. To illustrate how the approach can be used to include physical and geochemical complexities into reactive transport calculations, we have analysed the potential ingress of oxygenated glacial-meltwater in a heterogeneous fractured rock using the Forsmark site (Sweden) as an example. The results of high-performance reactive transport calculations show that, after a quick oxygen penetration, steady state conditions are attained where abiotic reactions (i.e. the dissolution of chlorite and the homogeneous oxidation of aqueous iron(II) ions) counterbalance advective oxygen fluxes. The results show that most of the chlorite becomes depleted in the highly conductive deformation zones where higher mineral surface areas are available for reactions.