Geological disposal and chemistry of high-level radioactive waste

Tachi, Yukio

Kagaku To Kyoiku, 71(10), p.420 - 423, 2023/10

no abstracts in English

Pore connectivity influences mass transport in natural rocks; Pore structure, gas diffusion and batch sorption studies

Yuan, X.*; Hu, Q.*; Lin, X.*; Zhao, C.*; Wang, Q.*; Tachi, Yukio; Fukatsu, Yuta; Hamamoto, Shoichiro*; Siitari-Kauppi, M.*; Li, X.*

Journal of Hydrology, 618, p.129172_1 - 129172_15, 2023/03

https://doi.org/10.1016/j.jhydrol.2023.129172

Effect of different interlayer counter-ions on montmorillonite swelling; Key controlling factors evaluated by molecular dynamic simulations

Yotsuji, Kenji*; Tachi, Yukio; Sakuma, Hiroshi*; Kawamura, Katsuyuki*

Genshiryoku Bakkuendo Kenkyu (CD-ROM), 29(2), p.63 - 81, 2022/12

https://doi.org/10.3327/jnuce.29.2_63

The understanding of the swelling phenomenon of montmorillonite is essential to predict the physical and chemical behavior of clay-based barriers in radioactive waste disposal systems. This study investigated the key factors controlling crystalline swelling behavior of montmorillonite with different interlayer counter-ions by molecular dynamics (MD) simulations. On the basis of the comparisons between MD simulated and experimental results, the water content in the interlayer in five homoionic (Na, K, Cs, Ca and Sr) montmorillonite was strongly correlated to the hydration number and the preference of an outer- or inner-sphere complex of each counter-ion. The detailed analysis for these results offer insights that the hydration number is controlled by the hydration free energy, the volume and the distribution of each interlayer counter-ion. The systematic MD simulations with virtually variable parameters clarified that the hydration free energy and the charge of interlayer counter- ions compete as influencing factors, and the control the formation rate of an outer-sphere complex of each counter-ion. The empirical relationships between these key factors will allow essential insights into predicting the swelling behavior of montmorillonite with different interlayer counter-ions.

Modelling of the LTDE-SD radionuclide diffusion experiment in crystalline rock at the sp Hard Rock Laboratory (Sweden)

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Keklinen, P.*; Hokr, M.*; ha, J.*; Vetenk, A.*; Reimitz, D.*; et al.

Geologica Acta, 20(7), 32 Pages, 2022/07

https://doi.org/10.1344/GeologicaActa2022.20.7

Task 9B of the SKB Task Force on Modelling of Groundwater Flow and Transport of Solutes in fractured rock focused on the modelling of experimental results from the LTDE-SD in situ tracer test performed at the sp Hard Rock Laboratory in Sweden. Ten different modelling teams provided results for this exercise, using different concepts and codes. Three main types of modelling approaches were used: (1) analytical solutions to the transport-retention equations, (2) continuum-porous-medium numerical models, and (3) microstructure-based models accounting for small-scale heterogeneity (i.e. mineral grains and microfracture distributions). The modelling by the different teams allowed the comparison of many different model concepts, especially in terms of potential zonations of rock properties (porosity, diffusion, sorption), such as the presence of a disturbed zone at the rock and fracture surface, the potential effects of micro- and cm-scale fractures.

Predictive modeling of a simple field matrix diffusion experiment addressing radionuclide transport in fractured rock. Is it so straightforward?

Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Iraola, A.*; Ebrahimi, K.*; Trinchero, P.*; Molinero, J.*; et al.

Nuclear Technology, 208(6), p.1059 - 1073, 2022/06

https://doi.org/10.1080/00295450.2021.1988822

The SKB Task Force is an international forum on modelling of groundwater flow and solute transport in fractured rock. The WPDE experiments are matrix diffusion experiments in gneiss performed at the ONKALO underground facility in Finland. Synthetic groundwater containing several conservative and sorbing tracers was injected along a borehole interval. The objective of Task 9A was the predictive modelling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches and codes, participated in this exercise. An important conclusion from this exercise is that the modelling results were very sensitive to the magnitude of dispersion in the borehole opening, which is related to the flow of water. Focusing on the tails of the breakthrough curves, which are more directly related to matrix diffusion and sorption, the results from the different teams were more comparable.

Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2021

Sugiura, Yuki; Suyama, Tadahiro*; Tachi, Yukio

JAEA-Data/Code 2021-017, 58 Pages, 2022/03

JAEA-Data-Code-2021-017.pdf:1.98MB

Sorption behavior of radionuclides (RNs) in buffer materials (bentonites), rocks and cementitious materials is one of the key processes in a safe geological disposal of radioactive waste because RNs migration in these materials is expected to be retarded by the sorption process. Therefore, it is necessary to understand the sorption process and develop a database compiling reliable data and mechanistic/predictive models so that reliable parameters can be set under a variety of geochemical conditions relevant to a performance assessment (PA). For this purpose, Japan Atomic Energy Agency (JAEA) has developed the database of sorption parameters in bentonites, rocks and cementitious materials. This sorption database (SDB) was firstly developed as an important basis for the H12 PA of a high-level radioactive waste disposal, and have been provided through the Web. JAEA has continued to improve and update the SDB in the view of potential future needs of data focusing on assuring the desired quality level and testing the usefulness of the databases for possible applications to the PA-related parameter setting. This report focuses on updating of the sorption database (JAEA-SDB) as a basis of integrated approach for the PA-related distribution coefficient (Kd) setting and development of mechanistic sorption models. This report also includes an overview of the database structure and contents. Kd data and their quality assurance (QA) results were updated from literature collected with wider ranges. As a result, 8,503 Kd data from 70 references related to the above-mentioned systems were added and the total number of Kd values in JAEA-SDB reached 79,072. The QA/classified Kd data reached about 75.4% for all Kd data in JAEA-SDB. The updated JAEA-SDB is expected to make it possible to give a basis for the next-step PA-related Kd setting.

Decrease of radionuclide sorption in hydrated cement systems by organic ligands; Comparative evaluation using experimental data and thermodynamic calculations for ISA/EDTA-actinide-cement systems

Ochs, M.*; Dolder, F.*; Tachi, Yukio

Applied Geochemistry, 136, p.105161_1 - 105161_11, 2022/01

https://doi.org/10.1016/j.apgeochem.2021.105161

Various types of radioactive wastes and environments contain organic substances that can stabilize the aqueous complexes with radionuclides and therefore lead to a decrease of sorption. The present study focuses on testing a methodology to quantify sorption reduction factors (SRFs) in the presence of organic ligands for cement systems. Three approaches for the estimation of SRFs; (1) analogy with solubility enhancement factors, (2) radionuclide speciation based on the thermodynamic calculations, and (3) experimental sorption data in ternary systems, were coupled and tested for the representative organic ligands (ISA and EDTA) and selected key radionuclides (actinides). Our approach allows to critically evaluate the dependence of SRFs for various systems on the chosen method of quantification, in accordance with the data availability for a given systems. The reliable SRFs can only be derived from the sorption measurements in ternary systems. SRF often need to be derived in the absence of such direct evidence, and estimations need to be made based on analogies and speciation information. However, such estimates may be subject to substantial uncertainties.

Evaluation report of Task 9C based on comparisons and analyses of modelling results for the ONKALO REPRO-TDE experiment

Soler, J. M.*; Keklinen, P.*; Pulkkanen, V.-M.*; Moreno, L.*; Iraola, A.*; Trinchero, P.*; Hokr, M.*; ha, J.*; Havlov, V.*; Trpkoov, D.*; et al.

SKB TR-21-09, 204 Pages, 2021/11

Diffusion of tritiated water, Cs, and I in compacted Ca-montmorillonite; Experimental and modeling approaches

Fukatsu, Yuta; Yotsuji, Kenji*; Okubo, Takahiro*; Tachi, Yukio

Applied Clay Science, 211, p.106176_1 - 106176_10, 2021/09

https://doi.org/10.1016/j.clay.2021.106176

The Impact of cement on argillaceous rocks in radioactive waste disposal systems; A Review focusing on key processes and remaining issues

Wilson, J.*; Bateman, K.; Tachi, Yukio

Applied Geochemistry, 130, p.104979_1 - 104979_19, 2021/07

https://doi.org/10.1016/j.apgeochem.2021.104979

The concept of deep geological disposal will include the multiple use of cement-based materials. In the case of argillaceous host rocks, the presence of hyperalkaline cement porefluid results in the destabilization of primary minerals in the argillite, resulting in the development of a zone of alteration at cement-rock interfaces. The process understanding gained from experimental, analogue, and modelling studies has been reviewed, and remaining areas of uncertainty identified. Although there is a reasonably good understanding of the mineral assemblages that are likely to occur due to cement-rock interactions, there are still some areas where a degree of uncertainty remains, in particular: the evolution of cement-argillite interfaces at T 25C; the rates at which secondary minerals form; the extent of pore clogging due to secondary mineral precipitation; the implications of alteration for radionuclide transport.