Reactive transport model of the long-term geochemical evolution in a HLW repository in granite at the disposal cell scale: Variants, sensitivities, and model simplifications

The assessment of the long-term performance of the engineered barrier systems of high-level radioactive waste (HLW) repositories requires the use of reactive transport models. Montenegro et al. (2023) presented a non-isothermal reactive transport model of the long-term geochemical evolution of a HLW disposal cell in a granitic host rock corresponding to a generic reference concept. The model accounted for the vitrified waste, the carbon-steel canister, the bentonite buffer and the reference granitic rock. Here we extend their model by considering model variants (V), sensitivity cases (SC) and model abstractions (MA). Variants V1, V2 and V3 consist of considering MX-80 bentonite instead of FEBEX bentonite (V1), a larger groundwater flux through the granite (V2) and the Czech reference crystalline rock as a host rock (V3). Cases SC1 and SC2 consider a decrease of the silica concentration threshold value in the glass dissolution rate (SC1) and an earlier canister failure time (SC2), respectively. Runs MA1 to MA4 consider smectite as an unreactive mineral phase (MA1), the porosity feedback effect on chemical and transport parameters (MA2), a time-varying corrosion rate (MA3), and a coarser finite element grid (MA4), respectively. Model results of V1 show a larger pH, a smaller precipitation of magnetite, siderite and greenalite and a slightly smaller dissolution of ISG and smectite than the base run of Montenegro et al. (2023). Model predictions are very sensitive to the increase in the groundwater flow through the granitic host rock (V2). However, predictions are not sensitive to the chemical composition of the granite porewater (V3). The decrease in the silica saturation threshold from 1·10 −3 to 5·10 −4 mol/L in SC1 leads to a significant decrease in glass dissolution. Glass dissolution after 50,000 years in SC2 (earlier canister failure) is much larger than that of the base run. Model results are not sensitive to considering smectite as an unreactive mineral phase (MA1). However, model results are very sensitive to the porosity feedback effect (MA2). A 60% volume fraction of Fe(s) remains uncorroded after 50,000 years when a variable corrosion rate is considered in MA3. In this case the precipitation of corrosion products is much smaller than that of the base run. The general patterns of the numerical results in MA4 (coarser grid) are similar to those of the base case. • Sensitivity analyses of of the long-term geochemical evolution of a HLW repository in granite are presented. • Predictions are very sensitive to an increase in groundwater flux through the granitic host rock. • Predictions are very sensitive to porosity feedback effect. Pore clogging prevents transport of corrosion products. • 80% of the canister remains uncorroded after 50,000 years when the corrosion rate depends on saturation index.

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Journal
Applied Geochemistry
Published
2024-10-05
DOI
https://doi.org/10.1016/j.apgeochem.2024.106188
Citations
5
Primary Topic
CO2 Sequestration and Geologic Interactions
Type
article
Field-Weighted Citation Impact
1.03

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article

Reactive transport model of the long-term geochemical evolution in a HLW repository in granite at the disposal cell scale: Variants, sensitivities, and model simplifications

Luís Montenegro, Javier Samper, Alba Mon
5 citations
Applied Geochemistry
CO2 Sequestration and Geologic Interactions
1.03
article

Reactive transport model of the long-term geochemical evolution in a HLW repository in granite at the disposal cell scale: Variants, sensitivities, and model simplifications

Luís Montenegro, Javier Samper, Alba Mon
article en
5 citations

Abstract

The assessment of the long-term performance of the engineered barrier systems of high-level radioactive waste (HLW) repositories requires the use of reactive transport models. Montenegro et al. (2023) presented a non-isothermal reactive transport model of the long-term geochemical evolution of a HLW disposal cell in a granitic host rock corresponding to a generic reference concept. The model accounted for the vitrified waste, the carbon-steel canister, the bentonite buffer and the reference granitic rock. Here we extend their model by considering model variants (V), sensitivity cases (SC) and model abstractions (MA). Variants V1, V2 and V3 consist of considering MX-80 bentonite instead of FEBEX bentonite (V1), a larger groundwater flux through the granite (V2) and the Czech reference crystalline rock as a host rock (V3). Cases SC1 and SC2 consider a decrease of the silica concentration threshold value in the glass dissolution rate (SC1) and an earlier canister failure time (SC2), respectively. Runs MA1 to MA4 consider smectite as an unreactive mineral phase (MA1), the porosity feedback effect on chemical and transport parameters (MA2), a time-varying corrosion rate (MA3), and a coarser finite element grid (MA4), respectively. Model results of V1 show a larger pH, a smaller precipitation of magnetite, siderite and greenalite and a slightly smaller dissolution of ISG and smectite than the base run of Montenegro et al. (2023). Model predictions are very sensitive to the increase in the groundwater flow through the granitic host rock (V2). However, predictions are not sensitive to the chemical composition of the granite porewater (V3). The decrease in the silica saturation threshold from 1·10 −3 to 5·10 −4 mol/L in SC1 leads to a significant decrease in glass dissolution. Glass dissolution after 50,000 years in SC2 (earlier canister failure) is much larger than that of the base run. Model results are not sensitive to considering smectite as an unreactive mineral phase (MA1). However, model results are very sensitive to the porosity feedback effect (MA2). A 60% volume fraction of Fe(s) remains uncorroded after 50,000 years when a variable corrosion rate is considered in MA3. In this case the precipitation of corrosion products is much smaller than that of the base run. The general patterns of the numerical results in MA4 (coarser grid) are similar to those of the base case. • Sensitivity analyses of of the long-term geochemical evolution of a HLW repository in granite are presented. • Predictions are very sensitive to an increase in groundwater flux through the granitic host rock. • Predictions are very sensitive to porosity feedback effect. Pore clogging prevents transport of corrosion products. • 80% of the canister remains uncorroded after 50,000 years when the corrosion rate depends on saturation index.

Applied GeochemistryVol. 175
Universidade da Coruña (ES)
Consellería de Cultura, Educación e Ordenación Universitaria, Xunta de Galicia, H2020 Euratom
Openalex Percentile: Top 26%
CO2 Sequestration and Geologic Interactions
1.03
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