Review about the Effect of He on the Microstructure of Spent Nuclear Fuel in a Repository

MRS Advances ◽  
2016 ◽  
Vol 1 (62) ◽  
pp. 4147-4156 ◽  
Author(s):  
C. Ferry ◽  
J. Radwan ◽  
H. Palancher
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Critical Concentration ◽  
Fuel Pellet ◽  
Spent Fuel ◽  
Operational Model ◽  
Matrix Microstructure ◽  
Natural Analogues ◽  
Order Of Magnitude ◽  
Radionuclide Release

ABSTRACTHelium is produced in spent nuclear fuel by α-decays of actinides. After 10,000 years, the concentration of He accumulated in UO2 spent fuel is about 0.23 at.%. For direct disposal of spent nuclear fuel, consequences of helium build-up on the fuel matrix microstructure must be evaluated since it can modify the radionuclide release when water comes into contact with the spent fuel surface, after breaching of the disposal canister. An operational model has been proposed in order to evaluate the effect of helium on the microstructure of spent fuel in a repository. Based on conservative assumptions and different scenarios of bubble population, the calculated helium critical concentration, that could lead to a partial loss of integrity of the spent fuel pellet, is 0.37 at.%. However, observations on He-implanted UO2, α-doped UO2 pellets and natural analogues evidence a macroscopic damage only for He concentrations, which are more than one order of magnitude higher.

Modelling the Activation of H2 on Spent Fuel Surface and Inhibiting Effect of UO2 Dissolution

2013 ◽  
Vol 1518 ◽  
pp. 133-138 ◽  
Author(s):  
L. Duro ◽  
O. Riba ◽  
A. Martínez-Esparza ◽  
J. Bruno
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Fuel Pellet ◽  
Dissolution Behavior ◽  
Dissolution Mechanism ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Secondary Phases ◽  
The Matrix ◽  
Fuel Storage

ABSTRACTThe dissolution of spent nuclear fuel is defined in two different time steps, i) the Instant Release Fraction (IRF) occurring shortly after water contacts the solid spent fuel and responsible of the fast release of those radionuclides that have been accumulated in the zones of the spent fuel pellet with low confinement, such as gap and grain boundaries and ii) the long term release of radionuclides confined in the spent fuel matrix, much slower and dependent on the conditions of the water that contacts the spent fuel.Several models have been developed to date to explain the dissolution behavior of spent nuclear fuel under disposal conditions. The Matrix Alteration Model (MAM) is one of the most evolved radiolytic models describing the dissolution mechanism in which an Alteration/Dissolution source term model is based on the oxidative dissolution of spent fuel. Under deep repository conditions and at the expected of water contacting time (after 1000 years of spent fuel storage), α radiation will be the main contributor to water radiolysis. In the current study, simulations evaluating the effect of surface area on the alteration/dissolution of spent fuel matrix are performed considering different particle sizes of spent fuel and simulations integrating the actinides dissolution have been performed considering the precipitation of secondary phases.

Operational Model for the Spent Nuclear Fuel Radionuclides Source Term in Presence of Water

2001 ◽  
Author(s):  
Christophe Poinssot ◽  
Christophe Jegou ◽  
Pierre Toulhoat ◽  
Jean-Marie Gras
Keyword(s):  
Nuclear Fuel ◽  
Closed System ◽  
Source Term ◽  
Spent Nuclear Fuel ◽  
Driving Forces ◽  
Spent Fuel ◽  
Microscopic Description ◽  
Operational Model ◽  
Geological Disposal ◽  
Source Term Model

Abstract Under the geological disposal conditions, spent fuel (SF) is expected to evolve during the 10,000 years while being maintained isolated from the biosphere before water comes in. Under those circumstances, several driving forces would lead to the progressive intrinsic transformations within the rod which would modify the subsequent release of radionuclides: the production of a significant volume of He, the accumulation of irradiation defects, the slow migration of radionuclides (RN) within the pellet. However, the current RN source terms for SF never accounted for these evolutions and was based on the existing knowledge on the fresh SF. Two major mechanisms were considered, the leaching of the readily available fraction (one which was supposed to be instantly accessible to water), and the release of RN through alteration of the UO2 grains. We are now proposing a new RN source term model based on a microscopic description of the system in order to also account for the early evolution of the closed system, the amplitude of which increases with the burnup and is greater for MOX fuels.

Kinetic Studies of Natural Uranium Minerals for the Long-Term Evolution of Spent Nuclear Fuel Under Oxidizing Conditions

1992 ◽  
Vol 294 ◽  
Author(s):  
Ignasi Casas ◽  
E. Cera ◽  
J. Bruno
Keyword(s):  
Spent Nuclear Fuel ◽  
Kinetic Studies ◽  
Natural Uranium ◽  
Spent Fuel ◽  
Natural Systems ◽  
Term Evolution ◽  
Natural Analogues ◽  
Order Of Magnitude ◽  
Granitic Groundwater

ABSTRACTThe time scale of spent fuel dissolution studies is of the order of magnitude of 2 to 10 years, while the performance of a spent fuel repository should be assessed for much longer times (105-106 years). These time scales can be bridged using appropriate natural analogues. Among other important information, the study of natural systems can give insight of which can be the oxidative alteration of spent fuel in granitic environments. However, in studying such systems, thermodynamic and kinetic data of relevant natural solid phases are needed.In this work we present preliminary results of dissolution experiments carried out under oxidizing conditions with selected and well characterized natural samples of the alteration chain of uraninite (i.e., uraninite, schoepite, uranophane).The experiments have been performed using a synthetic granitic groundwater as a leachant, in contact with air and at 25 °C.

Can Spent Nuclear Fuel Decay Heat Prevent Radionuclide Release?

2004 ◽  
Vol 824 ◽  
Author(s):  
James L. Jerden ◽  
Margaret M. Goldberg ◽  
James C. Cunnane ◽  
Theodore H. Bauer ◽  
Roald A. Wigeland ◽  
...  
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Radioactive Decay ◽  
Yucca Mountain ◽  
Spent Fuel ◽  
Decay Heat ◽  
Important Barrier ◽  
Water Accumulation ◽  
Radionuclide Release

AbstractHeat generated by radioactive decay of spent fuel represents a potentially important barrier to water accumulation on commercial spent nuclear fuel in breached waste packages. In the absence of water, fuel degradation and radionuclide release will be negligible. Thermal models for the proposed Yucca Mountain Repository suggest that, after a period of approximately 1000-4000 years (depending on loadingand ventilation conditions), the repository drift walls may decline to sub-boiling temperatures, thus allowing humidity in the drift to increase. The question thus arises, is the thermal gradient between the fuel and the drift sufficient to prevent water accumulation in a humid drift environment throughout the regulatory period? The answer depends on the balance between processes that oppose water condensation ontothe fuel (decay heat) and those that promote condensation such as the deliquescence of hygroscopic phaseswithin the fuel.Our experimental results indicate that deliquescence could lead to the condensation of water onto spent fuel despite the thermal “self-drying”effect if the following criteria are met: (1) the fission product salt CsI is present in the fuel or in the fuel-cladding gap, (2) the relative humidity in the driftexceeds 80% while temperatures in the waste package are around 90oC. Previous work suggests that these criteria may be met for some fuel pins within the proposed Yucca Mountain Repository. However,experiments that account for the role of U(VI) alteration phases suggest that deliquescence may be a self-limiting process in the sense that deliquescent components (e.g. Cs, Ba, Sr) may be incorporatedinto nondeliquescent U(VI) phases that form from the corrosion of spent fuel.

scholarly journals An Alternative Conceptual Model for the Spent Nuclear Fuel–Water Interaction in Deep Geologic Disposal Conditions

2021 ◽  
Vol 11 (18) ◽  
pp. 8566
Author(s):  
Barbara Pastina ◽  
Jay A. LaVerne
Keyword(s):  
Conceptual Model ◽  
Nuclear Fuel ◽  
Release Rate ◽  
Safety Assessment ◽  
Spent Nuclear Fuel ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Radiation Chemical ◽  
Radionuclide Release

For the long-term safety assessment of direct disposal of spent nuclear fuel in deep geologic repositories, knowledge on the radionuclide release rate from the UO2 matrix is essential. This work provides a conceptual model to explain the results of leaching experiments involving used nuclear fuel or simulant materials in confirmed reducing conditions. Key elements of this model are: direct effect of radiation from radiolytic species (including defects and excited states) in the solid and in the first water layers in contact with its surface; and excess H2 may be produced due to processes occurring at the surface of the spent fuel and in confined water volumes, which may also play a role in keeping the spent fuel surface in a reduced state. The implication is that the fractional radionuclide release rate used in most long-term safety assessments (10−7 year−1) is over estimated because it assumes that there is net UO2 oxidation caused by radiolysis, in contrast with the alternative conceptual model presented here. Furthermore, conventional water radiolysis models and radiation chemical yields published in the literature are not directly applicable to a heterogeneous system such as the spent fuel–water interface. Suggestions are provided for future work to develop more reliable models for the long-term safety assessment of spent nuclear fuel disposal.

Changes in spent nuclear fuel due to dry interim storage

2012 ◽  
Vol 1475 ◽  
Author(s):  
L. Duro ◽  
O. Riba ◽  
A. Martínez-Esparza ◽  
J. Bruno
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Initial Conditions ◽  
Critical Discussion ◽  
Fuel Pellet ◽  
Spent Fuel ◽  
Geological Repository ◽  
Irradiation Period ◽  
Interim Storage ◽  
Small Bubbles

ABSTRACTThe assessment of the main changes expected for spent nuclear fuel from its discharge to its deposition in a deep geological repository is of the outmost relevance to establish the initial conditions of the disposal. In this work, a literature review and a critical discussion of the main processes that will affect the structure and the inventory of the spent nuclear fuel during its interim dry storage is presented. Once the irradiation period is finished, the following changes are observed: i) the fuel pellet is fragmented due to the temperature gradient established during the irradiation stage. On average between 10-15 fragments are observed per pellet. ii) the initial gap existing between the pellet and the cladding decreases or disappears depending on the burnup. iii) a radial zonation is observed in the microstructure of the pellet. For burnup over 40MWd/KgU, the rim develops a porosity increase due to the high local burnup and the low temperature in the periphery. The rim also presents small bubbles of fission gases. This high burnup structure implies a degradation of the thermic conductivity in the pellet, that leads to a temperature increase in the center of the pellet with a subsequent migration of the fission gases and other impurities to the grain boundaries. The implications that all these changes may have on the spent fuel behaviour is presented and discussed.

scholarly journals Study on combustible gas generation and radionuclide release during underwater handling of the AM reactor spent fuel

2021 ◽  
Vol 7 (3) ◽  
pp. 223-229
Author(s):  
Artyom Z. Gayazov ◽  
Anton Yu. Leshchenko ◽  
Valery P. Smirnov ◽  
Pavel A. Ilyin ◽  
Vadim G. Teplov
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Chemical Interaction ◽  
Hydrogen Release ◽  
Spent Fuel ◽  
Gas Generation ◽  
Uranium Carbide ◽  
Combustible Gas ◽  
Combustible Gases ◽  
Radionuclide Release

Introduction. The paper addresses studies on the accumulation of combustible gases during underwater handling simulations for the leaky spent nuclear fuel from the AM reactor. Two fuel compositions were studied- uranium-molybdenum dispersed in magnesium and uranium carbide dispersed in calcium. Methods. The 137Cs release rate was measured during underwater storage of the uranium-molybdenum fuel. The kinetics of hydrogen release for both fuels and methane release for the carbide SNF were obtained. The kinetics approximate most with exponential dependences that formally correspond to first-order chemical reactions. A contribution of radiolytic hydrogen to the gases generated during the experiments was estimated. It was demonstrated that the determining source of the gases is the chemical interaction between the spent fuel and the water. The experiment with the uranium-molybdenum fuel demonstrated a pronounced passivation effect of the chemical processes on the fuel surface due to insoluble corrosion products. For the carbide SNF, an incubation period of about 20 hours was observed followed by an intensive release of hydrogen and methane. Results. The obtained results were subject to a comparative analysis against publications on the behavior of the fuel components in water. Conclusion. The findings can be applied to justify fire and explosion safety of underwater handling techniques for the damaged spent nuclear fuel with the considered fuel compositions (the spent fuel from reactors AM, AMB, EGP-6, etc.), e.g., to justify underwater preparations of the AMB spent fuel for reprocessing.

Chemical Effects at the Reaction Front in Corroding Spent Nuclear Fuel

2006 ◽  
Vol 985 ◽  
Author(s):  
Jeffrey A. Fortner ◽  
A. Jeremy Kropf ◽  
James L. Jerden ◽  
James C. Cunnane
Keyword(s):  
Transition Zone ◽  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Aqueous Environment ◽  
Spent Fuel ◽  
Aqueous Corrosion ◽  
Reduction Potentials ◽  
Chemical Effects ◽  
Before And After ◽  
X Ray Absorption

AbstractPerformance assessment models of the U. S. repository at Yucca Mountain, Nevada suggest that neptunium from spent nuclear fuel is a potentially important dose contributor. A scientific understanding of how the UO2 matrix of spent nuclear fuel impacts the oxidative dissolution and reductive precipitation of Np is needed to predict the behavior of Np at the fuel surface during aqueous corrosion. Neptunium would most likely be transported as aqueous Np(V) species, but for this to occur it must first be oxidized from the Np(IV) state found within the parent spent nuclear fuel. In this paper we present synchrotron x-ray absorption spectroscopy and microscopy findings that illuminate the resultant local chemistry of neptunium and plutonium within uranium oxide spent nuclear fuel before and after corrosive alteration in an air-saturated aqueous environment. We find the Pu and Np in unaltered spent fuel to have a +4 oxidation state and an environment consistent with solid-solution in the UO2 matrix. During corrosion in an air-saturated aqueous environment, the uranium matrix is converted to uranyl (UO22+) mineral assemblage that is depleted in Np and Pu relative to the parent fuel. The transition from U(IV) in the fuel to a fully U(VI) character across the corrosion front is not sharp, but occurs over a transition zone of ∼ 50 micrometers. We find evidence of a thin (∼ 20 micrometer) layer that is enriched in Pu and Np within a predominantly U(IV) environment on the fuel side of the transition zone. These experimental observations are consistent with available data for the standard reduction potentials for NpO2+/Np4+ and UO22+/U4+ couples, which indicate that Np(IV) may not be effectively oxidized to Np(V) at the corrosion potential of uranium dioxide spent nuclear fuel in air-saturated aqueous solutions.

scholarly journals The Need for Integrating the Back End of the Nuclear Fuel Cycle in the United States of America

MRS Advances ◽  
2018 ◽  
Vol 3 (19) ◽  
pp. 991-1003 ◽  
Author(s):  
Evaristo J. Bonano ◽  
Elena A. Kalinina ◽  
Peter N. Swift
Keyword(s):  
United States ◽  
Nuclear Fuel ◽  
United States Of America ◽  
Spent Nuclear Fuel ◽  
Fuel Cycle ◽  
Nuclear Fuel Cycle ◽  
The United States ◽  
Spent Fuel ◽  
Dry Storage ◽  
The Us

ABSTRACTCurrent practice for commercial spent nuclear fuel management in the United States of America (US) includes storage of spent fuel in both pools and dry storage cask systems at nuclear power plants. Most storage pools are filled to their operational capacity, and management of the approximately 2,200 metric tons of spent fuel newly discharged each year requires transferring older and cooler fuel from pools into dry storage. In the absence of a repository that can accept spent fuel for permanent disposal, projections indicate that the US will have approximately 134,000 metric tons of spent fuel in dry storage by mid-century when the last plants in the current reactor fleet are decommissioned. Current designs for storage systems rely on large dual-purpose (storage and transportation) canisters that are not optimized for disposal. Various options exist in the US for improving integration of management practices across the entire back end of the nuclear fuel cycle.

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