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At least 19 records

Impact of iron redox chemistry on nuclear waste disposal

For the safe disposal of nuclear waste, the ability to predict the changes in oxidation states of redox active actinide elements and fission products, such as U, Pu, Tc and Np is a key factor in determining their long term mobility. Both in the Geological Disposal Facility (GDF) near-field and in the far-field subsurface environment, the oxidation states of radionuclides are closely tied to changes in the redox condition of other elements in the subsurface such as iron. Iron pervades all aspects of the waste package environment, from the steel in the waste containers, through corrosion products, to the iron minerals present in the host rock. Over the long period required for nuclear waste disposal, the chemical conditions of the subsurface waste package will vary along the entire continuum from oxidizing to reducing conditions. This variability leads to the expectation that redox-active components such as Fe oxides can undergo phase transformations or dissolution; to understand and quantify such a system with respect to potential impacts on waste package integrity and radionuclide fate is clearly a serious challenge. Traditional GDF performance assessment models currently rely upon surface adsorption or single phase solubility experiments and do not deal with the incorporation of radionuclides into specific crystallographic sites within the evolving Fe phases. In this chapter, we focus on the iron-bearing phases that are likely to be present in both the near and far-field of a GDF, examining their potential for redox activity and interaction with radionuclides. To support this, thermodynamic and molecular modelling is particularly important in predicting radionuclide behaviour in the presence of Fe-phases. Examination of radionuclide contamination of the natural environment provides further evidence of the importance of Fe-phases in far-field processes; these can be augmented by experimental and analogue studies.

Environmental Molecular Sciences Laboratory↗

Effect of vanadium oxide addition on thermomechanical behaviors of borosilicate glasses: Toward development of high crack resistant glasses for nuclear waste disposal

The effect of of V2O5 additions (up to 8 mol%) on the physical properties (e.g., density, glass transition temperature and refractive indices) and mechanical behaviors (e.g., hardness, fracture toughness, elastic modulus) of a soda-lime borosilicate glass with a composition of 60.2SiO(2)-16.0B(2)O(3)-12.6Na(2)O-3.8Al(2)O(3)-5.7CaO-1.7ZrO(2) (mol%) have been investigated systematically. It was found that introducing V2O5 decreases the glass transition temperature and hardness while increases the refractive index and crack initiation load. Composition-property relationships, especially on mechanical properties, were examined in order to provide insights for the development of new glass materials with outstanding mechanical properties. The results show that V2O5 can be a glass component for engineering and insuring high crack resistant glasses and glasses with long-term stability. Additionally, elastic properties as a function of temperature were studied using Brillouin light scattering and temperature-independent elastic moduli behaviors were observed.

Lu, Xiaonan↗

International Approaches for Nuclear Waste Disposal in Geological Formations: Report on Fifth Worldwide Review

An important issue for present and future generations is the final disposal of spent nuclear fuel. Over the past over forty years, the development of technologies to isolate both spent nuclear fuel (SNF) and other high-level nuclear waste (HLW) generated at nuclear power plants and from production of defense materials, and low- and intermediate-level nuclear waste (LILW) in underground rock and sediments has been found to be a challenging undertaking. Finding an appropriate solution for the disposal of nuclear waste is an important issue for protection of the environment and public health, and it is a prerequisite for the future of nuclear power. The purpose of a deep geological repository for nuclear waste is to provide to future generations, protection against any harmful release of radioactive material, even after the memory of the repository may have been lost, and regardless of the technical knowledge of future generations. The results of a wide variety of investigations on the development of technology for radioactive waste isolation from 19 countries were published in the First Worldwide Review in 1991 (Witherspoon, 1991). The results of investigations from 26 countries were published in the Second Worldwide Review in 1996 (Witherspoon, 1996). The results from 32 countries were summarized in the Third Worldwide Review in 2001 (Witherspoon and Bodvarsson, 2001). The last compilation had results from 24 countries assembled in the Fourth Worldwide Review (WWR) on radioactive waste isolation (Witherspoon and Bodvarsson, 2006). Since publication of the last report in 2006, radioactive waste disposal approaches have continued to evolve, and there have been major developments in a number of national geological disposal programs. Significant experience has been obtained both in preparing and reviewing cases for the operational and long-term safety of proposed and operating repositories. Disposal of radioactive waste is a complex issue, not only because of the nature of the waste, but also because of the detailed regulatory structure for dealing with radioactive waste, the variety of stakeholders involved, and (in some cases) the number of regulatory entities involved.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Rock-welding materials development for deep borehole nuclear waste disposal

We report that various versions of deep borehole nuclear waste disposal have been proposed in the past in which effective sealing of a borehole after waste emplacement is generally required. In a high temperature disposal mode, the sealing function will be fulfilled by melting the ambient granitic rock with waste decay heat or an external heating source, creating a melt that will encapsulate waste containers or plug a portion of the borehole above a stack of the containers. However, there are certain drawbacks associated with natural materials, such as high melting temperatures, inefficient consolidation, slow crystallization kinetics, the resulting sealing materials generally being porous with low mechanical strength, insufficient adhesion to waste container surface, and lack of flexibility for engineering controls. In this study, we showed that natural granitic materials can be purposefully engineered through chemical modifications to enhance the sealing capability of the materials for deep borehole disposal. The present work systematically explores the effect of chemical modification and crystallinity (amorphous vs. crystalline) on the melting and crystallization processes of a granitic rock system. The approach can be applied to modify granites excavated from different geological sites. Several engineered granitic materials have been explored which possess significantly lower processing and densification temperatures than natural granites. Finally, those new materials consolidate more efficiently by viscous flow and accelerated recrystallization without compromising their mechanical integrity and properties.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

International Approaches for Nuclear Waste Disposal in Geological Formations: Report on Fifth Worldwide Review

The goal of the Fifth Worldwide Review is to document evolution in the state-of-the-art of approaches for nuclear waste disposal in geological formations since the Fourth Worldwide Review that was released in 2006. The last ten years since the previous Worldwide Review has seen major developments in a number of nations throughout the world pursuing geological disposal programs, both in preparing and reviewing safety cases for the operational and long-term safety of proposed and operating repositories. The countries that are approaching implementation of geological disposal will increasingly focus on the feasibility of safely constructing and operating their repositories in short- and long terms on the basis existing regulations. The WWR-5 will also address a number of specific technical issues in safety case development along with the interplay among stakeholder concerns, technical feasibility, engineering design issues, and operational and post-closure safety. Preparation and publication of the Fifth Worldwide Review on nuclear waste disposal facilitates assessing the lessons learned and developing future cooperation between the countries. The Report provides scientific and technical experiences on preparing for and developing scientific and technical bases for nuclear waste disposal in deep geologic repositories in terms of requirements, societal expectations and the adequacy of cases for long-term repository safety. The Chapters include potential issues that may arise as repository programs mature, and identify techniques that demonstrate the safety cases and aid in promoting and gaining societal confidence. The report will also be used to exchange experience with other fields of industry and technology, in which concepts similar to the design and safety cases are applied, as well to facilitate the public perception and understanding of the safety of the disposal approaches relative to risks that may increase over long times frames in the absence of a successful implementation of final dispositioning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Numerical evaluation of thermal effects from nuclear waste disposed in horizontal drillholes

© 2019 American Nuclear Society, Inc. We examine the temperature evolution near horizontal drillholes designed for the disposal of spent nuclear fuel and high-level radioactive waste. In this concept, directional drilling technology is used to complete a small-diameter, vertical access hole, which at the target depth gradually turns into a horizontal section dedicated for the end-to-end disposal of nuclear waste canisters in a suitable, low-permeable formation. Decay heat emanating from the waste leads to temperature increases within the drillhole and the surrounding host rock. Predicting the thermal evolution within the engineered and natural barrier systems is important, because high temperatures may lead to thermal stresses, alter material properties, or induce driving forces that affect the migration of radionuclides along the drillhole and in the near field of the repository. We present the results of numerical design calculations that examine the spatial and temporal evolution of temperature as a function of uncertain material properties and adjustable design parameters.

Finsterle, S↗

Thermal loading effects on chalk hydromechanical behavior for nuclear waste disposal

Safe disposal of heat-generating nuclear waste depends on host rock stability under thermal, hydrological, and mechanical stresses. This study investigates the effect of thermal loading on mechanical behavior of the shallowly buried Ghareb formation chalk through triaxial and hydrostatic constant strain rate and creep tests at temperatures up to 100 ˚C and effective pressures up to 20.7 MPa. Experimental results show that thermal loading reduces the elastic moduli of chalk by 50–75%, and a transition occurs above 60 ˚C where creep rates increase rapidly. Water saturation nearly doubles the thermally induced strain compared to dry conditions and strongly decreases material rigidity. Thermal loading also leads to significant pore pressure increases under undrained conditions and leads to reductions in the apparent permeability during drained conditions. Laboratory experimental data were used to parameterize and develop a preliminary constitutive model for predicting future deformation during repository operations in the Ghareb. The strongly coupled effects – mechanical weakening, fluid pressure fluctuations, and permeability modification – demonstrate that elevated repository temperatures will have a pronounced effect on the near field Ghareb behavior during waste disposal operations. The findings indicate that the coupled interactions must be considered in predictive models and repository design to ensure long-term nuclear waste isolation and safety.

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Thermophysical properties of the Ghareb formation relevant for nuclear waste disposal

The Ghareb formation, a shallowly buried porous chalk in Israel, is currently a candidate for nuclear waste disposal. The potential repository is somewhat unique for its host rock and emplacement in shallow (500 m) engineered large diameter boreholes. Herein, the thermal properties of the Ghareb are determined to support design and performance assessment; the relevant properties measured are thermal conductivity, specific heat capacity, thermal diffusivity, and thermal expansion coefficient along with their relationship with varying temperature. For the temperature range of 40 to 275 °C, the thermal conductivity ranges from 0.30 to 1.10 W/m·K, the thermal diffusivity ranges from 0.20 to 0.72 mm 2 /s, and volumetric heat capacity ranges from 0.86 to 2.00 MJ/m 3 ·K. Thermal strain measurements were used to estimate the linear thermal expansion coefficient to be 6·10 –4 –9·10 –2 °C -1 from 40 to 300 °C. These measured properties were used in a thermomechanical model to estimate near-field stresses an hour and 10 years after waste emplacement; the borehole was found to be stable. Thermal loading after 10 years was predicted to elevate local pore pressures by 1–1.5 MPa. The laboratory measurements coupled with analyses are the first attempts at performance assessment characterization for this first of its kind potential repository setting with this chosen host rock.

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Guiding Principles for Geochemical/Thermodynamic Model Development and Validation in Nuclear Waste Disposal: A Close Examination of Recent Thermodynamic Models for H + —Nd 3+ —NO 3 - (—Oxalate) Systems

Development of a defensible source-term model (STM), usually a thermodynamical model for radionuclide solubility calculations, is critical to a performance assessment (PA) of a geologic repository for nuclear waste disposal. Such a model is generally subjected to rigorous regulatory scrutiny. In this article, we highlight key guiding principles for STM model development and validation in nuclear waste management. We illustrate these principles by closely examining three recently developed thermodynamic models with the Pitzer formulism for aqueous H + —Nd 3+ —NO 3 - (—oxalate) systems in a reverse alphabetical order of the authors: the XW model developed by Xiong and Wang, the OWC model developed by Oakes et al., and the GLC model developed by Guignot et al., among which the XW model deals with trace activity coefficients for Nd(III), while the OWC and GLC models are for concentrated Nd(NO 3 ) 3 electrolyte solutions. The principles highlighted include the following: (1) Principle 1. Validation against independent experimental data: A model should be validated against experimental data or field observations that have not been used in the original model parameterization. We tested the XW model against multiple independent experimental data sets including electromotive force (EMF), solubility, water vapor, and water activity measurements. The results show that the XW model is accurate and valid for its intended use for predicting trace activity coefficients and therefore Nd solubility in repository environments. (2) Principle 2. Testing for relevant and sensitive variables: Solution pH is such a variable for an STM and easily acquirable. All three models are checked for their ability to predict pH conditions in Nd(NO 3 ) 3 electrolyte solutions. The OWC model fails to provide a reasonable estimate for solution pH conditions, thus casting serious doubt on its validity for a source-term calculation. In contrast, both the XW and GLC models predict close-to-neutral pH values, in agreement with experimental measurements. (3) Principle 3. Honoring physical constraints: Upon close examination, it is found that the Nd(III)-NO 3 association schema in the OWC model suffers from two shortcomings. Firstly, its second stepwise stability constant for Nd(NO 3 ) 2+ (log K 2 ) is much higher than the first stepwise stability constant for NdNO 3 2+ (log K 1 ), thus violating the general rule of (log K 2 –log K 1 ) < 0, or $\frac{K1}{K2}$>1. Secondly, the OWC model predicts abnormally high activity coefficients for Nd(NO 3 ) 2 + (up to ~900) as the concentration increases. (4) Principle 4. Minimizing degrees of freedom for model fitting: The OWC model with nine fitted parameters is compared with the GLC model with five fitted parameters, as both models apply to the concentrated region for Nd(NO 3 ) 3 electrolyte solutions. The latter appears superior to the former because the latter can fit osmotic coefficient data equally well with fewer model parameters. The work presented here thus illustrates the salient points of geochemical model development, selection, and validation in nuclear waste management.

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International Approaches for Nuclear Waste Disposal in Geological Formations: Geological Challenges in Radioactive Waste Isolation—Fifth Worldwide Review

The overall objective of the Fifth Worldwide Review (WWR-5) is to document the current state-of-the-art of major developments in a number of nations throughout the World pursuing geological disposal programs, and to summarize challenging problems and experience that have been obtained in siting, preparing and reviewing cases for the operational and long-term safety of proposed and operating nuclear waste repositories. The scope of the Review is to address current specific technical issues and challenges in safety case development along with the interplay of technical feasibility, siting, engineering design issues, and operational and post-closure safety. In particular, the chapters included in the report present the following types of information: the current status of the deep geological repository programs for high level nuclear waste and low- and intermediate level nuclear waste in each country, concepts of siting and radioactive waste and spent nuclear fuel management in different countries (with the emphasis of nuclear waste disposal under different climatic conditions and different geological formations), progress in repository site selection and site characterization, technology development, buffer/backfill materials studies and testing, support activities, programs, and projects, international cooperation, and future plans, as well as regulatory issues and transboundary problems.

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Numerical study of the chemo-mechanical behavior of FEBEX bentonite in nuclear waste disposal based on the Barcelona expansive model

Experimental studies show that compacted bentonite used as a backfill material for nuclear waste repository experiences strong coupling between chemical and mechanical processes. Here, we use a dual-structure expansive soil model, referred to as the Barcelona Expansive Model (BExM), to predict the behavior of bentonite buffer in subsurface emplacement tunnels for high-level radioactive waste. After emplacement, the bentonite is subjected to complex and coupled Thermal-Hydraulic-Mechanical-Chemical (THMC) processes. The BExM constitutive model is implemented in a multi-phase reactive transport and geomechanics simulator, TOUGHREACT-FLAC3D, and the model is verified with one benchmark test on FEBEX bentonite. We utilize a one-way Chemo-Mechanical (C-M) coupling approach, in which chemical changes affect the mechanical behavior of bentonite through the BExM linked with the evolution of mass fraction of smectite, exchangeable cation concentration, and ionic strength via osmotic suction. The parameters of the new coupled model for FEBEX bentonite are calibrated against a series of laboratory experiments with various salinity solutions. Finally, coupled THMC modeling is conducted for a generic argillite repository with bentonite buffer under high temperature, focusing on the long-term chemical change and its effect on the mechanical process.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Modeling nuclear waste disposal in crystalline rocks at the Forsmark and Olkiluoto repository sites – Evaluation of potential thermal–mechanical damage to repository excavations

We conduct coupled thermo-hydro-mechanical modeling of a KBS-3V repository design in crystalline rocks, using data and conditions from the Forsmark in Olkiluoto repository sites in Sweden and Finland. The study focuses on repository performance related to the impact of thermal and hydraulic evolution on the potential for thermal–mechanical damage to underground repository excavations. For the designs and conditions considered at the Forsmark and Olkiluoto repository sites, the simulations show a peak temperature well under the adopted performance target of a 100°C maximum temperature, whereas there is still a high potential for thermal–mechanical damage to the KBS-3V waste deposition holes. The thermal–mechanical damage is much more likely if rock permeability is so low that it delays saturation and swelling of bentonite-clay-based backfill beyond the time for the thermal–mechanical peak, which occurs 50 to 100 years after nuclear waste deposition. We also found that sidewalls of the KBS-3V emplacement tunnels are vulnerable to tensile fracturing due to the combined effect of thermal stressing and backfill swelling. The study highlights a strong interaction between bentonite-based backfill and host rock through capillary suction along with induced rock desaturation. A careful design and selection of the bentonite-clay-based backfill materials for KBS-3V tunnels and deposition holes can facilitate a timely saturation and backfill swelling that in turn can minimize thermal–mechanical damage.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Efficient Multi-Scale, Thermo-Hydro-Mechanical Numerical Model for Simulation of Long-Term Stability of Rooms for Nuclear Waste Disposal

This project demonstrated the feasibility of developing a numerical modeling tool that provides an efficient and unique approach to analyze the geomechanical performance of a deep geological repository (DGR) for high-level nuclear waste. The numerical modeling tool is physics-based and models the thermo-hydro-mechanical (THM) processes during the required time (up to one million years) for a DGR. The unique capability of the developed code is explicit representation of fracturing and a discrete fracture network (DFN) in the model that includes the entire repository layout for simulated time of one million years. Therefore, it can potentially address one of the challenges of analysis of a DGR, which is efficient numerical simulation of a multi-scale, physics-based models.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Individuals Who Build Solutions Across Boundaries for Environmental Remediation and Nuclear Waste Disposal - 16204

This paper profiles individuals who shifted from developing solutions primarily from within one organization to across multiple organizations for decisions requiring input from multiple parties. These individuals are engineers and scientists who work as government employees or government contractors. This paper contains six areas of discussion: 1. Why individuals build solutions across organizational boundaries, 2. The results they achieve, 3. Supporting skills and personal characteristics, 4. Means to build solutions across boundaries, 5. How they enlist others to participate, and 6. The importance of a catalyst. This paper is based on three sources of information. The primary source are interviews with nine engineers and scientists with direct experience building solutions across organizational boundaries in the fields of environmental remediation or nuclear energy/waste management and disposal. The second source are selected research studies. The third source is the author's experience both as a government employee and a consultant. The author's hope is that this paper will strengthen people's desire and ability to engage multiple parties in decisions requiring their input. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of a Radioactive Release in a Nuclear Waste Disposal Facility

The Waste Isolation Pilot Plant (WIPP) is a 655-meter deep mine near Carlsbad, New Mexico, used to dispose the nation’s defense transuranic waste. Limited airborne radioactivity was released from a container of radioactive waste in WIPP on 14 February, 2014. As designed, a mine ventilation filtration system prevented the large scale release of contamination from the underground. However, isolation dampers leaked, which allowed the release of low levels of contaminants after the event until they were sealed. None of the exposed individuals received any recordable dose. While surface contamination was limited, contamination in the ventilation system and portions of the underground was substantial. High efficiency particulate air (HEPA) filters in the operating ventilation system ensure continued containment during recovery and resumption of disposal operations. However, ventilation flow is restricted since the incident, with all exhaust air directed through the filters. Decontamination and natural fixation by the hygroscopic nature of the salt host rock has reduced the likelihood of further contamination spread. Contamination control and ventilation system operability are crucial for resumption of operations. This article provides an operational assessment and evaluation of these two key areas.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Advances in Thermal-Hydrologic Modeling of Nuclear Waste Disposal in Deep Boreholes - 16303

Deep borehole disposal is one of the potential options for safely isolating high-level radioactive waste. It is expected that existing drilling technology can provide reliable and cost-effective construction of suitable deep boreholes. In addition, favorable disposal conditions such as low permeability host rock, high salinity, and geochemically reducing conditions, exist at depth in many locations. Coupled thermal-hydrologic processes induced by heat from the radioactive waste may impact fluid flow and the associated migration of radionuclides. This work looks at those processes as was also done with recent studies. Simulations of thermal-hydrology for the emplacement of cesium and strontium capsules in a deep borehole are presented. The simulations looked at disposal options such as different disposal configurations and aging of waste to reduce thermal effects. The simulations studied temperature and fluid flux in the vicinity of the borehole. Simulation results include temperature and vertical flux profiles around the borehole at selected depths. Of particular importance are peak temperatures, and fluxes above the disposal zone. (authors)

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