The Influence of Ligands and Precipitates on the Release of Nuclides from the Near Field under Natural Repository Conditions

2000 ◽  
Vol 663 ◽  
Author(s):  
L. Liu ◽  
I. Neretnieks
Keyword(s):  
Uranium Oxide ◽  
Spent Nuclear Fuel ◽  
Transport Model ◽  
Radiation Power ◽  
Near Field ◽  
Reference Scenario ◽  
Spent Fuel ◽  
Secondary Phases ◽  
Fuel Surface ◽  
Fuel Pellets

ABSTRACTOnce groundwater intrudes into a damaged canister and wets the spent fuel pellets, radiation emitted from the spent nuclear fuel splits nearby water into oxidizing and reducing species. This may lead to an oxidizing condition near the fuel pellets. As a result, uranium oxide that makes up the fuel matrix will become more soluble, and the incorporated radionuclides will be released more rapidly. The dissolution process is, however, a dynamic one that can be influenced by many factors. Of great importance are the radiation power of the fuel matrix, the concentration of ligands near the fuel surface, and the transport resistance of the near field. Consequently, the escape of nuclides from the damaged canister is dominated mainly by the intrusion of ligands, and the precipitation/dissolution of secondary phases within the fuel rods. To investigate the possible effects of ligands and precipitates, a coupled dissolution and transport model, which includes the barrier effect of the Zircaloy claddings, is developed. The application of the model to a SKB-specified reference scenario indicates that by far the largest fraction of the oxidized uranium will reprecipitate within the canister. This may significantly decrease the fuel surface available for oxidation and the water available for radiolysis. Subsequently, much less fuel matrix will be dissolved and much less of the other nuclides will be released. Simulations further identify that carbonate and silicate have the greatest influences on the formation of secondary phases, and on the release of nuclides, under natural repository conditions.

Modeling spent nuclear fuel alteration and radionuclide migration in disposal conditions

2006 ◽  
Vol 94 (9-11) ◽  
Author(s):  
Laurent de Windt ◽  
H. Schneider ◽  
C. Ferry ◽  
H. Catalette ◽  
V. Lagneau ◽  
...  
Keyword(s):  
Reactive Transport ◽  
Spent Nuclear Fuel ◽  
Transport Model ◽  
Near Field ◽  
Radioactive Decay ◽  
Steel Corrosion ◽  
Spent Fuel ◽  
Fuel Pellets ◽  
Physico Chemical ◽  
Integrated Performance

A physico-chemical model developed for spent fuel alteration was integrated in a global reactive transport model of a spent fuel disposal system, considering both decaying and stable isotopes, corroded steel canisters, bentonite backfills and a clayey host-rock. Fuel evolution took into account radiolytic-enhanced corrosion and long-term solubility-controlled dissolution as well as instantaneous release fractions. The calculations show that spent-fuel dissolution has no significant alteration effect on the near-field components except an oxidizing plume in the vicinity of the waste packages. The dissolved uranyl species, partly precipitate as schoepite on the fuel pellets, and partly diffuse in the near-field where magnetite and pyrite reduce U(VI) to yield uraninite precipitation. Under disposal conditions, preliminary calculations indicate that steel corrosion may generate sufficient dissolved hydrogen as to react with radiolytic oxidants and inhibit fuel dissolution. The formation of a protective schoepite layer could also reduce the alteration of fuel pellets. Radionuclides migration (Am, Cs, I) in the near-field is discussed in a second stage discriminating between sorption, precipitation and radioactive decay processes. The migration of Cs is translated in terms of cumulative activity profiles useful for integrated performance assessment.

Reactive Transport Modeling of Radionuclide Source-Terms in an Underground Spent Fuel Disposal

2003 ◽  
Vol 807 ◽  
Author(s):  
L. De Windt ◽  
H. Catalette ◽  
J. M. Gras
Keyword(s):  
Reactive Transport ◽  
Transport Model ◽  
Near Field ◽  
Disposal Site ◽  
Spent Fuel ◽  
Fuel Pellets ◽  
Backfill Materials ◽  
Global Equilibrium ◽  
Stiff Clay ◽  
Failure Scenario

ABSTRACTThe reactive transport model HYTEC was used to simulate the migration over 100,000 years of cesium, americium and uranium released from spent fuel packages in the near-field components of an underground stiff clay disposal site. A global equilibrium thermodynamic approach including kinetic control of the spent fuel pellets was used with instantaneous release fractions and congruent dissolutions of the rim and the core zones. A failure scenario of the waste package after 10,000 years was considered with magnetite as the main corrosion product. The retention properties of magnetite and the different effects of bentonite and cementitious backfill materials were specifically analysed.

New insight studies of the secondary phase formation under repository conditions

MRS Advances ◽  
2020 ◽  
Vol 5 (11) ◽  
pp. 539-547
Author(s):  
N. Rodríguez-Villagra ◽  
L.J. Bonales ◽  
J. Cobos
Keyword(s):  
Raman Spectroscopy ◽  
Spent Nuclear Fuel ◽  
Near Field ◽  
Aqueous Media ◽  
Secondary Phase ◽  
Ambient Atmosphere ◽  
Secondary Phases ◽  
Γ Radiation ◽  
Radiation Fields ◽  
Groundwater Environment

ABSTRACTIn a deep geological repository (DGR) scenario, uranium oxidized in aqueous systems will be stabilized as UO22+ (hexavalent uranium), as a consequence of tetravalent uranium oxidation by radiolytic byproducts. Uranyl cationic species (UO22+) in different speciation forms are expected to be found at the whole pH range conditions. The importance of UO22+ lies in its potential incorporation of trace radioelements onto secondary uranyl phases. In view of the difficulty of U chemistry in natural groundwater, it is necessary to improve speciation assessment techniques so as to understand chemical processes. Raman spectroscopy has been shown as a powerful tool to analyze the speciation of various actinyl (UO22+,NpO2+ and PuO22+) and to determine the distribution of those elements which are more likely to be stable in a near-field groundwater environment. Therefore, the aim of this work is to follow UO22+ changes as a consequence of γ radiation in aqueous media under DGR conditions, and to understand the behavior of UO22+ as a function of aqueous media, which help to understand and predict the potential precipitation of the solid phases formed. In this work, the use of Raman spectroscopy adapted to the empirical analysis of different nuclear applications for initial uranium concentrations 0.04M at ambient atmosphere is shown, i.e. as monitoring tool for UO22+ precipitation as a function of pH, studying UO2(NO3)2·6H2O stability in aqueous solutions representative of groundwater, in particular at ionic strength I = 0.02 – 0.4 M and pH from 7 to 13.2; and to evaluate the effect of γ radiation fields. At 10−4-10-3 M of radiolytically formed H2O2 concentration, the amount of uranium in solution decreased, as a results of secondary phases precipitation. The results obtained will be useful to the performance assessment studies of the Spent Nuclear Fuel (SNF) stored in DGRs. The work performed provides a partial picture of secondary phase formations, as a result of corrosion of SNF in a DGR.

Zirconia Inert Matrix Fuel for Plutonium and Minor Actinides Management in Reactors and as an Ultimate Waste Form

2008 ◽  
Vol 1104 ◽  
Author(s):  
Claude Degueldre ◽  
Wolfgang Wiesenack
Keyword(s):  
Near Field ◽  
Fission Products ◽  
Minor Actinides ◽  
Spent Fuel ◽  
Geological Disposal ◽  
Inert Matrix Fuel ◽  
Inert Matrix ◽  
Fuel Pellets ◽  
Reducing Conditions ◽  
Deep Geological Disposal

AbstractA plutonia stabilised zirconia doped with yttria and erbia has been selected as inert matrix fuel (IMF) at PSI. The results of experimental irradiation tests on yttria-stabilised zirconia doped with plutonia and erbia pellets in the Halden research reactor as well as a study of zirconia solubility are presented. Zirconia must be stabilised by yttria to form a solid solution such as MAz(Y,Er)yPuxZr1-yO2-ζ where minor actinides (MA) oxides are also soluble. (Er,Y,Pu,Zr)O2-ζ (with Pu containing 5% Am) was successfully prepared at PSI and irradiated in the Halden reactor. Emphasis is given on the zirconia-IMF properties under in-pile irradiation, on the fuel material centre temperatures and on the fission gas release. The retention of fission products in zirconia may be stronger at similar temperature, compared to UO2. The outstanding behaviour of plutonia-zirconia inert matrix fuel is compared to the classical (U,Pu)O2 fuels. The properties of the spent fuel pellets are presented focusing on the once through strategy. For this strategy, low solubility of the inert matrix is required for geological disposal. This parameter was studied in detail for a range of solutions corresponding to groundwater under near field conditions. Under these conditions the IMF solubility is about 109 times smaller than glass, several orders of magnitude lower than UO2 in oxidising conditions (Yucca Mountain) and comparable in reducing conditions, which makes the zirconia material very attractive for deep geological disposal. The behaviour of plutonia-zirconia inert matrix fuel is discussed within a burn and bury strategy.

Modelling Oxidative Dissolution of Spent Fuel

1996 ◽  
Vol 465 ◽  
Author(s):  
Ivars Neretnieks
Keyword(s):  
Redox Reaction ◽  
Uranium Oxide ◽  
Reaction Rate ◽  
Spent Nuclear Fuel ◽  
Large Fraction ◽  
Reaction Rates ◽  
Spent Fuel ◽  
First Case ◽  
Rate Of Movement

ABSTRACTSpent nuclear fuel will, by the radiation, split nearby water into oxidizing and reducing compounds. The reducing compounds are mostly hydrogen that will diffuse away. The remaining oxidizing compounds can oxidize the uranium oxide of the fuel and make it more soluble. The oxidised uranium will dissolve and diffuse away. The nuclides previously incorporated in the spent fuel matrix can then be released and also migrate away from the fuel.A model is proposed where the produced oxidizing species compete for reaction with the fuel and for escaping out of the system. The chemical reaction rate of oxygen and fuel is taken from literature values based on experiments. The escape rate of oxidants to a receding redox front in the backfill is modelled assuming a redox reaction of oxidizing component and reducing component in the surrounding. The rate of movement of the redox front is determined from the rate of production of oxidants. This is estimated using a previously devised model that has been calibrated to in situ observed radiolysis.Three cases are modelled. In the first case it is assumed that the reducing compound is insoluble and that the reaction between oxygen and reducing mineral is very fast. In the second case it is assumed that the reducing component has a known solubility and that it can migrate to meet the oxygen and quickly react. In a third case a finite reaction rate is modelled between the oxygen and the reducing species.The sample calculations show that if the reducing mineral has to be supplied from the backfill a large fraction of the spent fuel could be oxidised. If the corrosion products of a degraded steel canister can supply the reducing species and the redox reaction is fast, very small amounts of the fuel could be oxidised. Literature data indicate that the redox reaction rate may not be so fast that it can be considered instantaneous and then a considerable fraction of the fuel could be oxidised. The model gives a means of exploring which mechanisms and data may be of most importance for radiolytic fuel dissolution, but the realism of the data and the model must be tested further. There is a lack of understanding and data on reaction rates, heterogeneous as well as homogeneous. This is crucial to the results.

Nuclear Waste

2014 ◽  
Author(s):  
Michael H. Fox
Keyword(s):  
Nuclear Power ◽  
Nuclear Reactor ◽  
Spent Nuclear Fuel ◽  
Nuclear Fission ◽  
Spent Fuel ◽  
Fuel Rods ◽  
Fuel Pellets ◽  
Water Filling ◽  
Nuclear Fuel Waste ◽  
Ranch House

I gazed over the railing into the crystal clear cooling pool glowing with blue Cherenkov light caused by particulate radiation traveling faster than the speed of light in water. I can see a matrix of square objects through the water, filling more than half of the pool. It looks like you could take a quick dip into the water, like an indoor swimming pool, but that would not be a good idea! It is amazing to think that this pool, about the size of a ranch house, is holding all of the spent fuel from powering the Wolf Creek nuclear reactor in Burlington, Kansas, for 27 years. The reactor was just refueled about a month before my visit, so 80 of the used fuel rod assemblies were removed from the reactor and replaced with new ones. The used fuel rods were moved underwater into the cooling pool, joining the approximately 1,500 already there. There is sufficient space for the next 15 years of reactor operation. There is no danger from standing at the edge of this pool looking in, though the levels of radon tend to be somewhat elevated and may electrostatically attach to my hard hat, as indeed some did. What I am gazing at is what has stirred much of the controversy over nuclear power and is what must ultimately be dealt with if nuclear power is to grow in the future—the spent nuclear fuel waste associated with nuclear power. What is the hidden danger that I am staring at? Am I looking at the unleashed power of Hephaestus, the mythical Greek god of fi re and metallurgy? Or is this a more benign product of energy production that can be managed safely? What exactly is in this waste? And is it really waste, or is it a resource? To answer that question, we have to understand the fuel that reactors burn. The fuel rods that provide the heat from nuclear fission in a nuclear reactor contain fuel pellets of uranium, an element that has an atomic number of 92 (the number of protons and also the number of electrons).

Near field evolution of a spent fuel repository in an argillaceous rock formation and impact on radionuclide migration

2020 ◽  
Author(s):  
Vanessa Montoya ◽  
Orlando Silva ◽  
Emilie Coene ◽  
Jorge Molinero ◽  
Renchao Lu ◽  
...  
Keyword(s):  
Ion Exchange ◽  
Radioactive Waste ◽  
Nuclear Fuel ◽  
Reactive Transport ◽  
Spent Nuclear Fuel ◽  
Near Field ◽  
Spent Fuel ◽  
Exchange Reactions ◽  
Radionuclide Migration ◽  
High Level

<p>In August 2015, the German government approved the national programme for the responsible and safe management of spent nuclear fuel (SNF) and radioactive waste proposed by the Federal Ministry for the Environment, Nature Conservation, Building and Reactor Safety (BMU). The assumption is that about ~ 1 100 storage casks (10 500 tons of heavy metal) in the form of spent fuel assemblies will be generated in nuclear power plants and will have to be disposed. However, a decision on the disposal concept for high-level waste is pending and an appropriate solution has to be developed with a balance in multiple aspects. All potential types of host rocks, clay and salt stones as well as crystalline formations are under consideration. In the decision process, evaluation of the risk of different waste management options and scenarios play an enormous role in the discussion. Coupled physical and chemical processes taking place within the engineered barrier system of a repository for high-level radioactive waste will define the radionuclide mobility/retention and the possible radiological impact. The objective of this work is to assess coupled processes occurring in the near-field of a generic repository for spent nuclear fuel in a high saline clay host rock, integrating complex geochemical processes at centimetre-scale. The scenario considers that radionuclides can be released during a period of thousands of years after full saturation of the bentonite barrier and the thermal phase.</p><p>Transport parameters and the discretization of the system, are implemented in a 2D axisymmetric geometry. The multi-barrier system is emplaced in clay and a solubility limited source term for the selected radionuclides is assumed. Kinetics and chemical equilibria reactions are simulated using parameters obtained from experiments. Additionally, porosity changes due to mineral precipitation/dissolution and feedback on the effective diffusion coefficient are taken into account. Protonation/deprotonation, ion exchange reactions and radionuclide inner-sphere sorption is considered.</p><p>Numerical simulations show, that, when the canister corrosion starts, the redox potential decreases, magnetite precipitates and H<sub>2</sub> is formed. Furthermore, the aqueous concentration of Fe(II) increases due to the presence of magnetite. By considering binding to montmorillonite via ion exchange reactions, the bentonite acts as a sink for Fe(II). Additionally, magnetite forms a chemical barrier offering significant sorption capacity for many radionuclides. Finally, a decrease of porosity in the bentonite/canister interface leads to a further deceleration of radionuclide migration. Due to the complexity of reactive transport processes in saline environments, benchmarking of reactive transport models (RTM) is important also to build confidence in those modelling approaches. Development of RTM benchmark procedures is part of the iCROSS project (Integrity of nuclear waste repository systems - Cross-scale system understanding and analysis) funded by both the Helmholtz Association and the Federal Ministry of Education and Research (BMBF).</p><p> </p>

Integrated Model of Korean Spent Fuel and High Level Waste Disposal Options

2009 ◽  
Author(s):  
Yongsoo Hwang ◽  
Ian Miller
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Fuel Cycle ◽  
Near Field ◽  
Integrated Model ◽  
High Level Waste ◽  
Spent Fuel ◽  
Parameter Uncertainties ◽  
Design Concepts ◽  
High Level

This paper describes an integrated model developed by the Korean Atomic Energy Research Institute (KAERI) to simulate options for disposal of spent nuclear fuel (SNF) and reprocessing products in South Korea. A companion paper (Hwang and Miller, 2009) describes a systems-level model of Korean options for spent nuclear fuel (SNF) management in the 21’st century. The model addresses alternative design concepts for disposal of SNF of different types (CANDU, PWR), high level waste, and fission products arising from a variety of alternative fuel cycle back ends. It uses the GoldSim software to simulate the engineered system, near-field and far-field geosphere, and biosphere, resulting in long-term dose predictions for a variety of receptor groups. The model’s results allow direct comparison of alternative repository design concepts, and identification of key parameter uncertainties and contributors to receptor doses.

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.

The influence of near field hydrogen on actinide solubilities and spent fuel leaching

2000 ◽  
Vol 88 (9-11) ◽  
Author(s):  
Kastriot Spahiu ◽  
L. Werme ◽  
U.-B. Eklund
Keyword(s):  
Experimental Study ◽  
Gas Phase ◽  
Hydrogen Pressure ◽  
Uranium Oxide ◽  
Near Field ◽  
Spent Fuel ◽  
Initial Amount ◽  
Temperature And Pressure ◽  
Corrosion Of Iron ◽  
Oxide Solubility

Large amounts of hydrogen are produced as a result of the anoxic corrosion of iron in the proposed container materials for some geologic repositories. Another hydrogen source, less important than the anoxic corrosion of iron, is the radiolysis of water by the spent fuel radiation. Gas phase formation occurs when the pressure of the hydrogen equals at least the hydrostatic pressure, around 5 MPa at 500 meters depth. The effects of 5 MPa hydrogen pressure on spent PWR fuel leaching and on uranium oxide solubility have been studied in carbonated solutions at 70 °C. The experiments were performed in a 1 liter autoclave, filled with 950 ml of a solution 10 mM NaCl, 2 mM NaHCOThe surface of spent fuel or U(IV) oxide is partially oxidized during storage, giving rise to relatively high levels of U(VI) in solution even during leaching in anoxic conditions. No such effect could be observed in the presence of 5 MPa hydrogen, indicating that this initial amount of U(VI) should have been reduced to U(IV). The experimental study of the influence of various parameters as temperature and pressure is still in progress.

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