A Review on the effect of iron on bentonite stability

Wilson, J.*; Sasamoto, Hiroshi; Tachi, Yukio; Kawama, Daisuke*

Applied Clay Science, 275, p.107862_1 - 107862_15, 2025/05

https://doi.org/10.1016/j.clay.2025.107862

High-Level Radioactive Waste (HLW) repositories include iron or steel-based containers/overpack and bentonite buffers. Over the last 25 years or so, research efforts have attempted to elucidate the nature of iron-bentonite interactions, especially the potential for the deleterious alteration of the swelling clay component (smectite), to iron-rich layer silicates, some of which lack the capacity for intracrystalline swelling. This could result in a reduction or loss in swelling pressure in the bentonite buffer which is designed to protect waste containers from shear forces and also acts to restrict water and solute transport, as part of an engineered barrier system. Most data on iron-bentonite interactions come from experimental and geochemical modelling studies, as natural analogue data are lacking. The data suggests that there is the potential for the development of an iron-rich bentonite alteration zone with smectite (generally present as the aluminous montmorillonite type) undergoing alteration to iron-rich solids, including layer silicates and steel corrosion products such as green rust or magnetite. The evidence available is complex, arguably incomplete, with many potential complex couplings. Many uncertainties remain despite efforts taken over the last 25 years, but plausible scenarios for iron-bentonite interactions have been identified and possible implications for buffer properties have been suggested.

Evolution of radionuclide transport and retardation processes in uplifting granitic rocks, Part 2; Modelling coupled processes in uplift scenarios

Metcalfe, R.*; Benbow, S. J.*; Kawama, Daisuke*; Tachi, Yukio

Science of the Total Environment, 958, p.177690_1 - 177690_17, 2025/01

https://doi.org/10.1016/j.scitotenv.2024.177690

Uplifting fractured granitic rocks occur in substantial areas of countries such as Japan. A repository site would be selected in such an area only if it is possible to make a safety case, accounting for the changing conditions during uplift. The safety case must include robust arguments that chemical processes in the rocks around the repository will contribute sufficiently to minimise radiological doses to biosphere receptors. To provide confidence in the safety arguments, numerical models need to be sufficiently realistic, but also parameterised conservatively (pessimistically). However, model development is challenging because uplift involves many complex couplings between groundwater flow, chemical reactions between water and rock, and changing rock properties. The couplings would affect radionuclide mobilisation and retardation, by influencing diffusive radionuclide fluxes between groundwater flowing in fractures and effectively immobile porewater in the rock matrix and radionuclide partitioning between water and solid phases, via: (i) mineral precipitation/dissolution; (ii) mineral alteration; and (iii) sorption/desorption. It is difficult to represent all this complexity in numerical models while showing that they are parameterised conservatively. Here we present a modelling approach, illustrated by simulation cases for some exemplar radioelements, to identify realistically conservative process conceptualisations and model parameterisations.

Thermodynamic properties and revised Helgeson-Kirkham-Flowers equations of state parameters of the hydrated and dehydrated monomeric silica species at = 0.01-600C, = 1-3000 bars, = 0.35-1.1 g cm, and = 0

Walker, C. S.*; Arthur, R. C.*; Anraku, Sohtaro; Sasamoto, Hiroshi; Mihara, Morihiro

Applied Geochemistry, 175, p.106086_1 - 106086_17, 2024/11

https://doi.org/10.1016/j.apgeochem.2024.106086

The thermodynamic properties and revised Helgeson-Kirkham-Flowers equation of state (r-H-K-F EoS) parameters of the hydrated (Si(OH)(aq), SiO(OH) and SiO(OH)) and fictive dehydrated (SiO(aq), HSiO and SiO) monomeric silicon species are used extensively to describe the pH, composition, temperature, and pressure dependence of formation/breakdown reactions of all silicon-bearing compounds globally. Experimental log10 equilbrium constant, K values describing the formation reactions of the hydrated and dehydrated monomeric silicon species were therefore compiled from the literature, extrapolated to zero ionic strength by specific ion interaction theory as required and used to derive their thermodynamic properties and r-H-K-F EoS parameters. Consideration of all formation reactions in the same study provides a collective, internally consistent update to the thermodynamic properties and r-H-K-F EoS parameters of the monomeric silicon species that can provide a satisfactory match to the experimental log10 K values at = 0.01-600C, = 1-3000 bars, = 0.35-1.1 g cm, and zero ionic strength. These temperature and pressure limits comfortably bracket t=0.01-100C and P =1-270 bars relecant to the geological disposal of radioactive wastes at depths of up to 1 km.

Structural characterization of C-A-S-H gels synthesized in different method using NMR

Hanamachi, Yuji*; Walker, C.*; Anraku, Sohtaro; Sasamoto, Hiroshi

NIMS Bisai Kozo Kaiseki Purattohomu Riyo Hokokusho (Internet), 4 Pages, 2024/10

no abstracts in English

Elasto-plastic mechanical analysis considering thermal and hydraulic effects for the in-situ experiment for full-scale engineered barrier system performance experiment at Horonobe Underground Research Laboratory

Ito, Shinji*; Shimizu, Hiroyuki*; Ono, Shintaro*; Takayama, Yusuke

Doboku Gakkai Rombunshu (Internet), 80(8), p.24-00030_1 - 24-00030_18, 2024/08

https://doi.org/10.2208/jscejj.24-00030

In the design consideration of a geological disposal facility for radioactive waste, it is essential to perform a mechanical evaluation that takes into account phenomena that may occur from construction and operation to post-closure. With this background, we have developed the long-term mechanical analysis system MACBECE. In this research, we have built an analysis system that can consistently evaluate the mechanical behavior considering the thermal and hydraulic evolution after the closure of the repository by incorporating the constitutive model for unsaturated soils and coupling with the thermal-hydraulic analysis. As a validation, a mechanical analysis was conducted for the in-situ experiment for full-scale engineered barrier system performance experiment at Horonobe URL. Despite some discrepancies due to constraints in two-dimensional analysis, the extended functionality of the analysis code was confirmed to effectively repro-duce the measured data.

Influence of temperature on stress corrosion cracking susceptibility of carbon steel in sodium hydrogen carbonate aqueous solution assuming upper limit of carbonate concentration in geological disposal environment

Takahashi, Rieko*; Taniguchi, Naoki

Zairyo To Kankyo, 73(6), p.153 - 163, 2024/06

https://doi.org/10.3323/jcorr.73.153

Carbon steel is one of the candidate materials for overpacks in geological disposal of high-level radioactive waste, and is known to susceptible to stress corrosion cracking(SCC) depending on the condition in carbonate environment. In order to understand the influence of temperature on the SCC susceptibility of carbon steel, slow strain rate test (SSRT) of rolled steel were performed in NaHCO aqueous solution with varying temperature in the range of 303-393K for conditions of 0.1-0.5 mol/dm, which is assumed to be the upper limit of carbonate concentration in groundwater in a geological disposal environment. As the results, no obvious influence of temperature on mechanical properties such as fracture strain ratio and reduction area ratio were observed, but SCC susceptibility based on SCC fracture ratio increased at relatively low temperatures of 303K and 323K. It was suggested that the reason for the higher SCC sensitivity at lower temperatures was due to slower repassivation at lower temperatures. Regarding the type of SCC, intergranular SCC was dominant at low temperatures and tended to transition to intergranular SCC at higher temperatures. Transgranular SCC tended to be observed at lower potentials than those at which intergranular SCC was observed.

Model catchments for testing biosphere assessment models of geological disposal

Yamaguchi, Masaaki; Suzuki, Yuji*; Kabasawa, Satsuki; Kato, Tomoko

JAEA-Data/Code 2024-001, 21 Pages, 2024/03

JAEA-Data-Code-2024-001.pdf:3.45MB
JAEA-Data-Code-2024-001-appendix(CD-ROM).zip:8.0MB

Model catchments have developed for use in testing various assessment models that can consider specific surface environmental conditions such as topography, riverine systems, and land use in the biosphere assessment of HLW geological disposal. The model catchments consist of the topography and riverine system of the catchment area created using existing tools, as well as land use and population distribution, river discharge, sediment flux data set by algorithms from topographical data. Datasets of three types of model watersheds (Types 1 to 3, watershed area: 730 to 770 km) with different topographical characteristics have released as raster data that can be handled by geographic information systems (GIS). Since the model catchments were created virtually reflecting as much as possible the main characteristics of Japan's surface environment, they can be used as a test bed for conducting hydraulic/mass transport analysis to set the GBI and compartment model.

NMR study of C-A-S-H structures

Hanamachi, Yuji*; Walker, C.*; Sasamoto, Hiroshi; Mihara, Morihiro

NIMS Bisai Kozo Kaiseki Purattofuomu Riyo Hokokusho (Internet), 2 Pages, 2023/12

A High-volume Fly ash Silica fume Cement (HFSC) has been considered as the use of concrete support of drift in deep disposal of radioactive wastes. JAEA has been carried out experiments and modeling studies to evaluate chemical stability of C-A-S-H gel synthesized which would be believed as the dominant component of the HFSC. For the modeling purpose, it is necessary to evaluate the chemical composition both of C-A-S-H gel synthesized and accompanied minerals in the experiment. In the year of 2020, Al and Si NMR measurement were performed to identify Al and Si distribution in the sample and chemical composition of C-A-S-H gel was derived. However, it was impossible to derive the C-A-S-H gel composition having the expected Al/Si molar ratio since there were several accompanied minerals produced in the experiment due to the short term of immersion. This time similar approach to derive C-A-S-H gel composition is adopted using NMR measurement for the sample of longer time (6 months).

Geological disposal and chemistry of high-level radioactive waste

Tachi, Yukio

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

https://doi.org/10.20665/kakyoshi.71.10_420

no abstracts in English

Secondary consolidation characteristic of bentonite by long-term consolidation tests of 2.7, 3.7 and 4 years

Takayama, Yusuke; Yamamoto, Yoichi*; Goto, Takahiro*

Jiban Kogaku Janaru (Internet), 18(3), p.317 - 330, 2023/09

https://doi.org/10.3208/jgs.18.317

It has been reported that the deformation greatly increased in the secondary consolidation process in the past long-term consolidation test of 1.8 years on Na-type bentonite/sand mixed soil. Therefore, we analyzed potential contributing factors in this behavior. A long-term consolidation test for about 10 years on bentonite and kaolinite was started using the test equipment with countermeasures against these factors. In this paper, the secondary consolidation behavior of bentonite was investigated based on the long-term consolidation test data for 2.7, 3.7 and 4 years. The results were generally consistent with the conventional findings on soil mechanics that the deformation due to secondary consolidation progresses linearly with respect to logarithm of time. This test will be continued for about 10 years and longer-term secondary consolidation behavior will be investigated.