Reactive transport modeling in fractured media of nuclear glass for industrial application

Abstract : Understanding the alteration of nuclear glass in a fracture network of a vitrified glass block is important for the safe conditioning of nuclear waste (quantification of the risks associated with radionuclide release). Performance assessment of geological nuclear waste repositories entails modelling of the long-term evolution of the fractured nuclear glass block aqueous alteration, because the considered time scale, of several thousands of years, is beyond the range of any direct experimental perspectives. This dissertation aims then to bridge the gap between the reservoir-scale flow and transport simulations and the micron-scale modeling of the glass-water interfacial processes, by bringing the quantitative evaluation of the glass aqueous degradation at the block scale.To tackle this issue, the main objectives of this thesis were fixed as follows: (i) reproduction of the experimental results previously obtained (for some fractures modeled in a discrete way in the diffusive mode),(ii) analysis of the impact of fractures geometries on the quantity of altered glass at the scale of some fractures modeled in a discrete way, (iii) investigation of the possibilities of the geochemical model adaptation for the equivalent homogenous modeling, (iv) establishment of a methodology for glass block fracture network characterization, (v) geostatistical and geometric modeling, (vi) calculation of the equivalent diffusive, hydraulic and glass dissolution kinetics controlling properties and (vii) upcoming reactive transport modeling at the scale of one canister.As an illustrative example, the proposed image processing-based fracture network characterization methodology was applied to two-dimensional (2D) high-resolution images of two blocks of vitrified glass. This application brought into service both hard data obtained by direct measurement of the fracture network and soft physics-based explanatory data and resulted in the creation of multiple realizations of fracture network equivalent tessellation that were further used as physical representation for the calculation of the equivalent hydraulic, diffusive, and alteration kinetics - controlling properties. The evolution of the quantity of altered glass obtained by conducting reactive transport modeling applied to several realizations of the equivalent fracture network tessellation was compared with the experimental data of the aqueous alteration test of a non-radioactive full-scale nuclear glass canister. The results show that implementation of the devised procedure presents an opportunity for better understanding the impact of fracturing on aqueous alteration of borosilicate glass and provides a reliable tool enabling different scenarios of repository evolution to be accounted for.
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Maria Repina. Reactive transport modeling in fractured media of nuclear glass for industrial application. Ecology, environment. PSL Research University, 2019. English. ⟨NNT : 2019PSLEM007⟩. ⟨tel-02309222⟩

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