| 1. |
- Iraola, Aitor, et al.
(författare)
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Microtomography-based Inter-Granular Network for the simulation of radionuclide diffusion and sorption in a granitic rock
- 2017
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Ingår i: Journal of Contaminant Hydrology. - : Elsevier BV. - 0169-7722 .- 1873-6009. ; 207, s. 8-16
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 2. |
- Schmidt, H., et al.
(författare)
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Gamma and pulsed electron radiolysis studies of CyMe 4 BTBP and CyMe 4 BTPhen: Identification of radiolysis products and effects on the hydrometallurgical separation of trivalent actinides and lanthanides
- 2021
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Ingår i: Radiation Physics and Chemistry. - : Elsevier BV. - 1879-0895 .- 0969-806X. ; 189
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Tidskriftsartikel (refereegranskat)abstract
- The radiolytic stability of the highly selective ligands CyMe4BTBP and CyMe4BTPhen against ionizing gamma radiation was studied in 1-octanol solution. CyMe4BTBP and CyMe4BTPhen are important extractants for a potential treatment of used nuclear fuel. They were studied under identical experimental conditions to directly compare the effects of gamma and pulsed electron radiolysis on the ligands and systematically study the influence of structural changes in the ligand backbone. Distribution ratios of Am3+, Cm3+ and Eu3+, the residual concentration of CyMe4BTBP and CyMe4BTPhen in solution, and the formation of radiolysis products were studied as a function of absorbed gamma dose and presence of an acidic aqueous phase during irradiation. Quantitative and semi-quantitative analyses were used to elucidate the radiolysis mechanism for both ligands. Addition products of alpha-hydroxyoctyl radicals formed through radiolysis of the 1-octanol diluent to the ligand molecules were identified as the predominant radiolysis products. These addition products also extract trivalent metal ions, as distribution ratios remained high although the parent molecule concentrations decreased. Therefore, the utilization time of a solvent using these extractants under the harsh conditions of used nuclear fuel treatment could be considerably longer than expected. Understanding the radiolysis mechanism is crucial for designing more radiation resistant extractants.
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| 3. |
- Soler, Josep, et al.
(författare)
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Modelling of the LTDE-SD radionuclide diffusion experiment in crystalline rock at the Aspo Hard Rock Laboratory (Sweden)
- 2022
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Ingår i: Geologica Acta. - : Universitat Autònoma de Barcelona. - 1695-6133 .- 1696-5728. ; 20, s. 1-32
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 4. |
- Trinchero, Paolo, et al.
(författare)
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Upscaling of radionuclide transport and retention in crystalline rocks exhibiting micro-scale heterogeneity of the rock matrix
- 2020
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Ingår i: Advances in Water Resources. - : Elsevier BV. - 0309-1708 .- 1872-9657. ; 142
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Tidskriftsartikel (refereegranskat)abstract
- In different in-situ diffusion experiments carried out in fractured crystalline rocks, sorbing radionuclides have shown a behaviour that strongly differs from what is predicted by homogeneous-based models. Their breakthrough curves are in fact often characterised by a fast first-arrival and these radionuclides can penetrate surprisingly long distances deep into the matrix. The heterogeneous structure of mineral distribution and porosity geometry had been offered as an explanation for these discrepancies. Here, we use reactive transport simulations to investigate the effect of the sparse distribution of sorption sites on the breakthrough curves of sorbing radionuclides. At small scale, the computed breakthrough curves significantly differ from those predicted using homogeneous models. For instance, the early part of these curves does not show any clear separation with the corresponding part of the curve of a non-sorbing tracer and a long transition zone is observed, with a very smooth slope of the tailing. Two different upscaling strategies, aimed at propagating the signal of heterogeneous retention over larger scales, are proposed and demonstrated against independent solutions computed at intermediate scales. The upscaling strategies are also used to show that at large scales (e.g. the scale of interest in a safety assessment study for a deep geological repository for nuclear waste) the signature of mineralogical heterogeneity is smoothed out and the heterogeneous breakthrough curve is well approximated by a homogeneous solution where the radionuclide distribution coefficient for the pure mineral phase is scaled by the mineral volume fraction. However, the spatial persistence of the heterogeneous signature is significant when the sorbing mineral is present in a low amount.
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