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.

Horonobe Underground Research Laboratory Project Investigation Report for the 2023 Fiscal Year

Nakayama, Masashi

JAEA-Review 2024-042, 111 Pages, 2024/11

JAEA-Review-2024-042.pdf:7.83MB

The Horonobe Underground Research Laboratory (URL) Project is being pursued by the Japan Atomic Energy Agency (JAEA) to enhance the reliability of relevant technologies for geological disposal of high-level radioactive waste through investigating the deep geological environment within the host sedimentary rocks at Horonobe Town in Hokkaido, north Japan. In the fiscal year 2023, we continued R&D on "Study on near-field system performance in geological environment", "Demonstration of repository design options", and "Understanding of buffering behaviour of sedimentary rock to natural perturbations". These are identified as key R&D on challenges to be tackled in the Horonobe underground research plan for the fiscal year 2020 onwards. Specifically, "full-scale engineered barrier system (EBS) performance experiment" and "solute transport experiment with model testing" were carried out as part of "Study on nearfield system performance in geological environment". "Demonstration of engineering feasibility of repository technology" and "evaluation of EBS behaviour over 100C" were addressed for "Demonstration of repository design options". The validation of a method for assessing permeability using the Ductility Index and a method for estimating the state of in-situ ground pressure from hydraulic perturbation tests were investigated as part of the study "Understanding of buffering behaviour of sedimentary rock to natural perturbations". In FY2023, we resumed construction of the subsurface facilities, 3 new tunnels in the 350 m gallery and resumed excavation of the East Access Shaft and the Ventilation Shaft. By the end of FY2023, the 350 m gallery extension (tunnel extension 66 m) had been completed, and the depths of the East Access Shaft and Ventilation Shaft were GL-424 m and GL-393 m respectively.

Trial analysis of chemical behavior in high-level radioactive liquid waste tank at accident of evaporation to dryness by boiling of reprocessing plant

Yoshida, Kazuo; Hiyama, Mina*; Tamaki, Hitoshi

JAEA-Research 2024-007, 24 Pages, 2024/08

JAEA-Research-2024-007.pdf:2.1MB

An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. It has been observed experimentally that volatility of RuO is suppressed by HNO generated by HNO radiolysis. The analysis of chemical reactions of NO including HNO and HNO in the waste tank is essential to simulate of these phenomena. To resolve this issue, an analytical approach has been attempted to couple dynamically two computer codes SHAWED and SCHERN. The simulation of boiling behavior in the tank is conducted with SHAWED. SCHERN simulates chemical behaviors of HNO, HNO and NO in the tank. A programmatic coupling algorithm and a trial simulation of the accident are presented in this report.

Horonobe Underground Research Laboratory Project; Investigation program for the 2023 fiscal year

Nakayama, Masashi

JAEA-Review 2023-019, 70 Pages, 2023/11

JAEA-Review-2023-019.pdf:6.83MB

The Horonobe Underground Research Laboratory (URL) Project is being pursued by the Japan Atomic Energy Agency (JAEA) to enhance the reliability of relevant technologies for geological disposal of high-level radioactive waste through investigating the deep geological environment within the host sedimentary rocks at Horonobe Town in Hokkaido, north Japan. In the fiscal year 2023, we continue R&D on "Study on near-field system performance in geological environment", "Demonstration of repository design options", and "Understanding of buffering behaviour of sedimentary rocks to natural perturbations". These are identified as key R&D challenges to be tackled in the Horonobe underground research plan for the fiscal year 2020 onwards. In the "Study on near-field system performance in geological environment", we conduct the coupled analysis on the full-scale engineered barrier system performance experiment and test the coupled simulation code through comparison with different simulation codes in the international DECOVALEX-2023 collaboration project. Borehole investigations are also carried out for solute transport experiments in the Koetoi Formation. As for "Demonstration of repository design concept", we carry out in situ experiments and data analysis on concrete deterioration under the subsurface conditions. Geophysical surveys are also carried out around an experimental tunnel to be newly excavated at the 350m gallery and characterise the initial conditions of the excavation damaged zone. For the "Understanding of buffering behaviour of sedimentary rocks to natural perturbations", we analyse the results of the hydraulic disturbance tests conducted in previous years and understand the relationship between rock stress / stress state and fault / fracture hydraulic connectivity. Concerning the construction and maintenance of the subsurface facilities, the 350 m gallery is extended and shafts are sank to a depth of 500 m.

Impact of MOX fuel use in light-water reactors; Long-term radiological consequences of disposal of high-level waste in a geological repository

Minari, Eriko*; Kabasawa, Satsuki; Mihara, Morihiro; Makino, Hitoshi; Asano, Hidekazu*; Nakase, Masahiko*; Takeshita, Kenji*

Journal of Nuclear Science and Technology, 60(7), p.793 - 803, 2023/07

https://doi.org/10.1080/00223131.2022.2146016

Development of simulation program; SHAWED for analysis of accident of evaporation to dryness by boiling of reprocessed high level liquid waste in tank

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2022-011, 37 Pages, 2022/12

JAEA-Research-2022-011.pdf:2.88MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents at a fuel reprocessing plant. Two major mechanisms are expected for fission products (FPs) transfer from liquid to vapor phase. One is non-volatiles FPs transfer in the form of mists to the vapor phase in the tank, the other is volatilization of such as Ruthenium. These FPs transferred to the vapor phase in the tank could be released with water and nitric-acid mixed steam and NO gas flow to the environment. NO is generated from denitration of nitrate fission products during dry out phase. These phenomena occurred in this accident originate from the liquid waste boiling in the tank. It is essential for the risk assessment of this accident to simulate thermo-hydraulic and chemical behaviors in the waste tank quantitatively with a versatile computer program. The SHAWED (imulation of igh-level radioctive aste vaporation and ryness) has been developed to realize these requirements. In this report, detailed description of major analytical models is explained based on the features of this accident, and some simulation examples are also described for the use in an actual risk assessment.

Horonobe Underground Research Laboratory Project; Investigation report for the 2021 fiscal year

Nakayama, Masashi

JAEA-Review 2022-025, 164 Pages, 2022/11

JAEA-Review-2022-025.pdf:12.25MB

The Horonobe Underground Research Laboratory (URL) Project is being pursued by the Japan Atomic Energy Agency (JAEA). The main aim of this project is to enhance the reliability of relevant disposal technologies for geological disposal of high-level radioactive waste through a comprehensive research and development (R&D) program in the deep geological environment within the host sedimentary rock at Horonobe in Hokkaido, north Japan. In fiscal year 2021, we continued R&D on three important issues specified in the "Horonobe Underground Research Plan from Fiscal Year 2020", which involve "Study on near-field system performance in geological environment", "Demonstration of repository design options", and "Understanding of buffering behaviour of sedimentary rock to natural perturbations". Specifically, "full-scale engineered barrier system (EBS) performance experiment" and "solute transport experiment with model testing" were carried out as part of "Study on near-field system performance in geological environment". "Demonstration of engineering feasibility of repository technology" and "evaluation of EBS behaviour over 100C' were addressed for "Demonstration of repository design options". A study on "Understanding of buffering behaviour of sedimentary rock to natural perturbations" was also implemented in two areas, "evaluation of intrinsic buffering against endogenic and exogenic processes" and "development of techniques for evaluating excavation damaged zone (EDZ) self-sealing behaviour after backfilling". The results of the R&D, along with those obtained in other departments of JAEA, will reinforce the technical basis for both repository implementation and safety regulation. For the sake of this, we will steadily proceed with this project in collaboration with relevant organizations and universities both domestically and internationally and also widely publish the plans and results of the R&D to ensure their transparency and technical reliability.

Horonobe Underground Research Laboratory Project; Investigation report for the 2020 fiscal year

Nakayama, Masashi

JAEA-Review 2021-053, 133 Pages, 2022/02

JAEA-Review-2021-053.pdf:14.45MB

The Horonobe Underground Research Laboratory (URL) Project is being pursued by the Japan Atomic Energy Agency (JAEA). The main aim of this project is to enhance the reliability of relevant disposal technologies for geological disposal of high-level radioactive waste through a comprehensive research and development (R&D) program in the deep geological environment within the host sedimentary rock at Horonobe in Hokkaido, north Japan. In fiscal year 2020, JAEA continued R&D on three important issues specified in the "Horonobe Underground Research Plan from Fiscal Year 2020", which involve "Study on nearfield system performance in geological environment", "Demonstration of repository design options", and "Understanding of buffering behavior of sedimentary rock to natural perturbations". Specifically, 'full scale engineered barrier system (EBS) experiment' and 'solute transport experiment' were carried out as part of "Study on near-field system performance in geological environment". 'Development and testing of EBS emplacement / retrieval and tunnel closure technologies' and 'evaluation of EBS behavior over 100C' were addressed for "Demonstration of repository design options". A study on "Understanding of buffering behavior of sedimentary rock to natural perturbations" was also implemented in two areas, 'evaluation of hydromechanical responses of faults to water pressure changes' and 'development of techniques for evaluating self-sealing behavior of an excavation damaged zone after backfilling'. The results of the R&D, along with those obtained in other departments of JAEA, will reinforce the technical basis for both repository implementation and safety regulation. For the sake of this, JAEA will steadily proceed with this project in collaboration with relevant organizations and universities both domestically and internationally and also widely publish the plans and results of the R&D to ensure their transparency and technical reliability.

Analysis of behavior of Ru with nitrogen oxide chemical behavior in accident of evaporation to dryness by boiling of reprocessed high level liquid waste

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2021-005, 25 Pages, 2021/08

JAEA-Research-2021-005.pdf:2.91MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. To resolve this issue, an empirical correlation equation of Ru mass transfer coefficient across the vapor-liquid surface, which can be useful for quantitative simulation of Ru mitigating behavior, has been obtained from data analyses of small-scale experiments conducted to clarify gaseous Ru migrating behavior under steam-condensing condition. A simulation study has been also carried out with a hypothetical typical facility building successfully to demonstrate the feasibility of quantitative estimation of amount of Ru migrating in the facility using the obtained correlation equation implemented in SCHERN computer code which simulates chemical behaviors of nitrogen oxide based on the condition also simulated thermal-hydraulic computer code.

Horonobe Underground Research Laboratory Project; Investigation program for the 2021 fiscal year

Nakayama, Masashi

JAEA-Review 2021-009, 54 Pages, 2021/07

JAEA-Review-2021-009.pdf:5.02MB

The Horonobe URL Project is being pursued by the JAEA to enhance the reliability of relevant disposal technologies for geological disposal of High-level Radioactive Waste through investigations of the deep geological environment within the host sedimentary rock at Horonobe Town in Hokkaido, north Japan. In 2021 fiscal year (2021/2022), JAEA continue to conduct research on "Demonstration of EBS in geological environment", "Demonstration of disposal concept", and "Validation of buffer capacity of the sedimentary rock to tectonism", which are the important issues shown in the Horonobe underground research plan after 2020 fiscal year. The main studies to be conducted in 2021 fiscal year are as follows. As "Demonstration of EBS in geological environment", we will shift to the test under the condition that the influence of heating is eliminated in the full scale EBS experiment. As "Demonstration of disposal concept", as a demonstration of the closure techniques, it details the conditions under which long-term transitions in the tunnel and surrounding bedrock have a significant impact on safety assessments. And we will continue engineering scale experiment to confirm the workability and performance of plugs and laboratory tests to examine the interaction between backfilling materials and buffer materials. As "Validation of buffer capacity of the sedimentary rock to tectonism", we will analyze the results of the hydraulic disturbance test and continue to study the hydraulic disconnection of faults/fissures in the Wakkanai Formation. As an advancement of technology for investigating and evaluating areas where the flow of groundwater is extremely slow, a boring exploration will be conducted to confirm the three-dimensional distribution of the fossil seawater area.