The behavior of unirradiated UO2and uraninite under repository conditions characterized by Raman

MRS Advances ◽  
2016 ◽  
Vol 1 (62) ◽  
pp. 4157-4162 ◽  
Author(s):  
L. J. Bonales ◽  
J.M. Elorrieta ◽  
C. Menor-Salván ◽  
J. Cobos
Keyword(s):  
Raman Spectroscopy ◽  
Spent Nuclear Fuel ◽  
Secondary Phase ◽  
Storage Conditions ◽  
Oxidation Products ◽  
Deep Geological Repository ◽  
Secondary Phases ◽  
Secondary Phase Formation ◽  
Geological Repository ◽  
Spectroscopy Studies

ABSTRACTRaman spectroscopy studies have been performed on one hand to identify different materials related to spent nuclear fuel (SNF), and on the other hand to study the behavior of SNF at different storage conditions. Specifically, the expected oxidation of the SNF matrix under dry storage conditions and the formation of secondary phases (SP), as a result of corrosion of SNF in a deep geological repository, have been studied. In order to perform these experiments, two protocols based on the Raman spectroscopy technique have been developed. The results show U4O9/U3O7and U3O8as oxidation products of UO2powder at high temperatures in air, and the secondary phase formation (rutherfordine, UO2(CO3), soddyite, (UO2)2SiO4•2H2O, uranophane alpha Ca(UO2)2(SiO3OH)2•5H2O and kasolite, PbUO2SiO4•H2O), due to uraninite corrosion under the conditions of Sierra Albarrana (Spain).

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.

Modelling Radionuclide Mobility of Spent Fuel in a Deep Geological Repository Located in a Clay Bedrock

2009 ◽  
Author(s):  
Lara Duro ◽  
Abel Tamayo ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza
Keyword(s):  
Source Term ◽  
Spent Nuclear Fuel ◽  
Near Field ◽  
Radioactive Decay ◽  
Secondary Phase ◽  
Diffusive Transport ◽  
Deep Geological Repository ◽  
Spent Fuel ◽  
Geological Repository ◽  
Source Term Model

Source term models are widely used to assess the behaviour of spent nuclear fuel after final disposal. However, most models do not take into account some phenomena which are expected to control the transport of radionuclides through the near field. Some uncertainties arise from this fact, thus making it difficult to obtain proper simulations of radionuclide behaviour in the near field. In this work, we have used a compartmental code to build up an integrated source term model in an attempt to overcome the abovementioned drawbacks. The model developed takes into account radiolytically-mediated matrix dissolution, radioactive decay chains, diffusive transport, and retardation by sorption and secondary phase precipitation, among other processes. In addition, this model has been used to estimate radionuclide mobility from spent fuel located in a conceptual clay geological repository.

The Effect of Bromide on Oxygen Yields in Homogeneous α-radiolysis

MRS Advances ◽  
2017 ◽  
Vol 2 (13) ◽  
pp. 711-716 ◽  
Author(s):  
Lovisa Bauhn ◽  
Christian Ekberg ◽  
Patrik Fors ◽  
Kastriot Spahiu
Keyword(s):  
Radiation Field ◽  
Spent Nuclear Fuel ◽  
Radiation Doses ◽  
Deep Geological Repository ◽  
Spent Fuel ◽  
Mass Spectrometric Measurement ◽  
Α Decay ◽  
Geological Repository ◽  
Dissolved Ions ◽  
Dissolved Hydrogen

ABSTRACTIn a scenario where ground water enters a canister for spent nuclear fuel in a deep geological repository, the presence of dissolved ions in the water could possibly influence the fuel dissolution due to effects on radiolysis yields. One species of particular interest in this context is bromide, which has a proven ability to scavenge hydroxyl radicals much faster than molecular hydrogen does. As a result, bromide could inhibit the beneficial effect of dissolved hydrogen, which has been shown in γ-radiolysis experiments. However, already a few hundred years after repository closure, α-decay starts to dominate in the radiation field from the spent fuel. Hence, the effects of α-radiolysis are expected to govern the fuel dissolution over the geological timeframes of the repository. In the present work, α-radiolysis experiments have been performed to determine the effect of bromide ions on the yield of hydrogen peroxide by mass spectrometric measurement of its decomposition product oxygen. The use of high activity 238Pu solutions has made it possible to study this effect during pure α-radiolysis from a homogeneously distributed radiation field. To simulate deep bedrock repository conditions, and to minimize the influence of in-leaking O2 from air, the studies were performed using graphite sealed stainless steel autoclaves with an initial atmosphere of 10 bar H2. The results show that addition of 1 mM Br- to the solution gives no significant effect on the O2 yield for radiation doses up to 2 MGy. This lack of effect is most likely explained by the limited radical escape yields from radiation tracks in pure α-radiolysis.

scholarly journals Assessment of the climate changes evolution for the long-term safety of the radioactive waste repository in the Czech Republic

2019 ◽  
Vol 133 ◽  
pp. 02005
Author(s):  
Markéta Camfrlová
Keyword(s):  
Czech Republic ◽  
Radioactive Waste ◽  
Spent Nuclear Fuel ◽  
Global Climate ◽  
Deep Geological Repository ◽  
Climatic Effects ◽  
The Czech Republic ◽  
Area Of Interest ◽  
Geological Repository

Nuclear energy accounts for a significant part of the total energy production in the Czech Republic, which is currently facing a problem dealing with the high-level radioactive waste (HLW) and the spent nuclear fuel (SNF). Deep repository is the safest option for storage of HLW. Rock environment of the area must guarantee the stability of the deep geological repository for at least 100,000 years. The aim of the research is a long-term evaluation of the climatic changes of the hypothetical area of interest, which corresponds to the candidate sites for deep geological repository in the Czech Republic. The occurrences of endogenous and exogenous phenomena, which could affect site stability, were evaluated. Concerning exogenous processes, research focuses mainly on the assessment of climatic effects. The climate scenarios for the Central Europe were examined – global climate change, glaciation, and the depth of permafrost as well as CO2 increase.

scholarly journals In situ nuclear-glass corrosion under geological repository conditions

2019 ◽  
Vol 3 (1) ◽  
Author(s):  
Mathieu Debure ◽  
Yannick Linard ◽  
Christelle Martin ◽  
Francis Claret
Keyword(s):  
Pure Water ◽  
Secondary Phase ◽  
Predictive Modelling ◽  
Diffusion Experiment ◽  
Secondary Phases ◽  
Glass Corrosion ◽  
Geological Repository ◽  
High Level ◽  
Rock Supports

Abstract Silicate glasses are durable materials but laboratory experiments reveal that elements that derive from their environment may induce high corrosion rates and reduce their capacity to confine high-level radioactive waste. This study investigates nuclear-glass corrosion in geological media using an in situ diffusion experiment and multi-component diffusion modelling. The model highlights that the pH imposed by the Callovo–Oxfordian (COx) claystone host rock supports secondary-phase precipitation and increases glass corrosion compared with pure water. Elements from the COx rock (mainly Mg and Fe) form secondary phases with Si provided by the glass, which delay the establishment of a passivating interface. The presence of elements (Mg and Fe) that sustain glass alteration does not prevent a significant decrease in the glass-alteration rate, mainly due to the limited species transport that drives system reactivity. These improvements in the understanding of glass corrosion in its environment provide further insights for predictive modelling over larger timescales and space.

PH3 Effects on the Electrochemical Degradation of SOFC Anode

2011 ◽  
Author(s):  
Huang Guo ◽  
Gulfam Iqbal ◽  
Bruce S. Kang
Keyword(s):  
Electrochemical Performance ◽  
Secondary Phase ◽  
Anode Surface ◽  
Electrochemical Degradation ◽  
Secondary Phases ◽  
Nickel Phosphate ◽  
Secondary Phase Formation ◽  
Cell Anode ◽  
Fuel Cell Anode ◽  
Ppm Level

Solid Oxide Fuel Cell anode is readily degraded by trace amount of Phosphine (PH3) contaminant that is found in coal-derived syngas. PH3 interacts with the anode material and affects its electrochemical performance by forming secondary phases. In this paper, the influence of the ppm level of PH3 with moisture is investigated on the formation of secondary phases and hence on anode electrochemical performance degradation. Nickel yttria-stabilized zirconia (Ni-YSZ) anode shows immediate and severe electrochemical degradation due to PH3 in moist hydrogen condition attributed to the nickel-phosphate secondary phase formation. Whereas in dry hydrogen condition, nickel-phosphide is preferred to form on the anode surface that shows less deleterious effects on SOFC performance as compared to nickel-phosphate.

Identification of Secondary Phases Formed During Unsaturated Reaction of UO2 with EJ-13 Water

1989 ◽  
Vol 176 ◽  
Author(s):  
J. K. Bates ◽  
B. S. Tani ◽  
E. Veleckis ◽  
O. J. Wronklewicz
Keyword(s):  
Phase Formation ◽  
Secondary Phase ◽  
Yucca Mountain ◽  
Solution Chemistry ◽  
Spent Fuel ◽  
Secondary Phases ◽  
Secondary Phase Formation

ABSTRACTA set of experiments, wherein UO2 has been contacted by dripping water, has been conducted over a period of 182.5 weeks. The experiments are being conducted to develop procedures to study spent fuel reaction under unsaturated conditions that are expected to exist over the lifetime of the proposed Yucca Mountain repository site. One half of the experiments have been terminated, while one half are ongoing. Analyses of solutions that have dripped from the reacted UO2 have been performed for all experiments, while reacted UO2 surfaces have been examined for the terminated experiments. A pulse of uranium release from the UO2 solid, combined with the formation of schoepite on the surface of the UO2, was observed between 39 and 96 weeks of reaction. Thereafter, the uranium release decreased and a second set of secondary phases was observed. The latter phases incorporated cations from the EJ-13 water and include boltwoodite, uranophane, sklodowskite, compreignacite, and schoepite. The experiments are continuing to monitor whether additional changes in solution chemistry or secondary phase formation occurs.

Flaw Acceptance Evaluation for the Final Disposal Canister Under Earthquake Induced Rock Shear

2019 ◽  
Author(s):  
Hsoung-Wei Chou ◽  
Szu-Ying Wu
Keyword(s):  
Crack Detection ◽  
Spent Nuclear Fuel ◽  
Global Model ◽  
Deep Geological Repository ◽  
Element Analysis ◽  
Final Disposal ◽  
Shear Loads ◽  
Buffer Material ◽  
Geological Repository ◽  
Loading Case

Abstract When a canister used for final disposal of spent nuclear fuel is in the deposition hole of deep geological repository, the loading case which would most impact the structure integrity of the canister is to postulate an earthquake induced rock shear through a deposition hole. This paper evaluates the acceptable sizes of defects in the cast iron insert of canister using fracture mechanics analysis. The submodelling technique of finite element analysis was employed to calculate the fracture behavior of the canister with postulated defects subjected to shear loads due to earthquake. At first, the stresses of the global model and the uncracked submodel were compared to check the correctness of the transferred displacements from the global model to the submodel. Then, surface and internal flaws with various shapes and depths were modeled individually in the submodel. A 5 cm shear displacement was applied on buffer and then transmitted to the canister. The calculations of J-integral of each flaw indicate that the surface semi-elliptical defect is more critical and the density of buffer material significantly affects the acceptable size of postulated defects. Present results can provide acceptance criteria of crack detection for canisters during manufacture and examination processes.

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