Effect of Water Radiolysis Caused by Dispersed Radionuclides on Oxidative Dissolution of Spent Fuel in a Final Repository

2001 ◽  
Vol 135 (2) ◽  
pp. 154-161 ◽  
Author(s):  
Jinsong Liu ◽  
Ivars Neretnieks
Keyword(s):  
Water Radiolysis ◽  
Spent Fuel ◽  
Oxidative Dissolution ◽  
Effect Of Water

Modeling of the Effects of Radiolysis on UO2-dissolution Employing Recent Experimental Data

2003 ◽  
Vol 807 ◽  
Author(s):  
Mats Jonsson ◽  
Fredrik Nielsen ◽  
Ella Ekeroth ◽  
Trygve E. Eriksen
Keyword(s):  
Experimental Data ◽  
Uranium Dioxide ◽  
Kinetic Data ◽  
Experimental Results ◽  
Recent Experimental Data ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Inhibiting Effect ◽  
Effect Of Water ◽  
Radiolysis Products

ABSTRACTThis study examines the effect of water radiolysis on the dissolution of uranium dioxide. A model is created to describe the system of uranium dioxide fragments in water, and the production and reactions of radiolysis products (using recent kinetic data). The system is evaluated under different conditions using MAKSIMA-CHEMIST. Conditions examined include presence of carbonate in the water and effects of hydrogen. The simulations are compared to experimental results on spent fuel dissolution. Surprisingly, the simulated U(VI)-release agrees within a factor of three with the experimentally found U(VI)-release. The inhibiting effect of hydrogen is clearly demonstrated by the simulations. From the results of the simulations we are also able to conclude that the main inhibiting effect of H2 is the reaction with OH• and not the reduction of U(VI) to U(IV).

On the Role of H2 as an Inhibitor of UO2 Matrix Dissolution

2007 ◽  
Author(s):  
Juan Merino ◽  
Xavier Gaona ◽  
Lara Duro ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza
Keyword(s):  
Chemical Composition ◽  
Partial Pressure ◽  
Water Radiolysis ◽  
Water Interface ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Term Stability ◽  
Long Term Stability

The study of spent fuel behaviour under disposal conditions is usually based on conservative approaches assuming oxidising conditions produced by water radiolysis at the fuel/water interface. However, the presence of H2 from container corrosion can inhibit the dissolution of the UO2 matrix and enhance its long-term stability. Several studies have confirmed the decrease in dissolution rates when H2 is present in the system, although the exact mechanisms of interaction have not been fully established. This paper deals with a radiolytic modelling exercise to explore the consequences of the interaction of H2 with radicals generated by radiolysis in the homogeneous phase. The main conclusion is that in all the modelled cases the presence of H2 in the system leads to a decrease in matrix dissolution. The extent of the inhibition, and the threshold partial pressure for the inhibition to take place, both depend in a complex way on the chemical composition of the water and the type of radiation present in the system.

Modelling the Release of Radionuclides from the Spent Fuel and their Transport in the Near Field: a Coupled Approach

2003 ◽  
Vol 807 ◽  
Author(s):  
Juan Merino ◽  
Esther Cera ◽  
Jordi Bruno ◽  
Aurora Martínez-Esparza
Keyword(s):  
Near Field ◽  
Radioactive Decay ◽  
Secondary Phase ◽  
Coupled System ◽  
Integrated Approach ◽  
Integrated Systems ◽  
Advective Transport ◽  
Spent Fuel ◽  
Oxidative Dissolution ◽  
Phase Precipitation

ABSTRACTIn this work we have developed a model for the release of radionuclides from the spent fuel coupled with their transport through the near field. A compartmental approach has been used, as this methodology is well suited to model integrated systems. Several processes have been taken into account: oxidative dissolution of the spent fuel matrix, radioactive decay and chains, diffusive and advective transport, retardation by sorption and secondary phase precipitation. Results illustrate the complex evolution of the radionuclide concentrations in the gap and the near field. Hence, the main conclusion from this study is the requirement to model this coupled system using a compartmental integrated approach.

Spent fuel alteration model integrating processes of different time-scales

MRS Advances ◽  
2020 ◽  
Vol 5 (3-4) ◽  
pp. 159-166
Author(s):  
O. Riba ◽  
E. Coene ◽  
O. Silva ◽  
L. Duro
Keyword(s):  
Reactive Transport ◽  
Transport Model ◽  
Beta Radiation ◽  
Comsol Multiphysics ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Subsequent Reduction ◽  
Reactive Transport Model ◽  
Safety Assessments ◽  
Different Time Scales

ABSTRACTA 1D reactive transport model has been implemented in iCP (interface COMSOL Multiphysics and PhreeqC) to assess the corrosion of Spent Fuel (SF), considered as homogeneous UO2(am,hyd) doped with Pd. The model couples: i) generation of water radiolysis species by alpha and beta radiation considering the complete water radiolysis system with the kinetic reactions involving: H+, OH-, O2, H2O2, H2, HO2-, HO2·, O·, O-, O2-, H·, ·OH and e- ii) processes occurring in the spent fuel surface: oxidative dissolution reactions of UO2(am,hyd) and subsequent reduction of oxidized fuel, considering H2 activation by Pd, and iii) corrosion of Fe(s) in oxic and anoxic conditions. Process i) has been implemented in COMSOL and processes ii) and iii) have been implemented in PHREEQC with their kinetic constants being calibrated with different sets of experimental data published in the open literature. The model yields a UO2(am,hyd) dissolution rates similar to the values selected in safety assessments.

Mechanisms governing the release of radionuclides from spent nuclear fuel in geological repository: major outcomes of the European Project SFS

2006 ◽  
Vol 932 ◽  
Author(s):  
Christophe Poinssot ◽  
Cécile Ferry ◽  
Bernd Grambow ◽  
Manfred Kelm ◽  
Kastriot Spahiu ◽  
...  
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Kinetic Scheme ◽  
Water Radiolysis ◽  
Large Set ◽  
Spent Fuel ◽  
Fuel Performance ◽  
Geological Repository ◽  
The Matrix ◽  
Release Model

ABSTRACTEuropean Commission supported a wide research project entitled “Spent Fuel Stability under repository conditions” (SFS) within the 5th FWP, the aim of which was to develop a common understanding of the radionuclides release from spent nuclear fuel in geological disposal and build a RN release model in order to assess the fuel performance. This project achieved by the end of 2004 focuses both on the Instant Release Fraction (IRF) model and the Matrix Alteration Model (MAM).A new IRF model was developed based on the anticipated performances of the various fuel microstructures (gap, rim, grains boundaries) and the potential diffusion of RN before the canister breaching. However, this model lets the choice to the end-user about the degree of conservativeness to consider.In addition, fuel alteration has been demonstrated to be linked to the production of radiolytic oxidants by water radiolysis at the fuel interface, the oxidation of the fuel interface by radiolytic oxidants and the subsequent release of uranium under the influence of aqueous ligands. A large set of experimental data was therefore acquired in order (i) to upgrade the current radiolytic kinetic scheme, (ii) to experimentally correlate the fuel alteration rate and the fuel specific alpha activity by performing experiments on alpha doped samples, (iii) to experimentally test the potential inhibitor effect of hydrogen on fuel dissolution. Based on these results, a new MAM was developed, which was also calibrated using the experiments on inactive UO2 samples. This model was finally applied to representative granitic, salt and clayey environment to predict spent fuel long-term fuel performance.

Study of the Consequences of Secondary Water Radiolysis within and Surrounding a Defective Canister

2000 ◽  
Vol 663 ◽  
Author(s):  
Jinsong Liu ◽  
Bo Strömberg ◽  
Ivars Neretnieks
Keyword(s):  
Near Field ◽  
Experimental Studies ◽  
Solubility Limit ◽  
Balance Model ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Secondary Minerals ◽  
First Case ◽  
Bentonite Buffer

ABSTRACTA model has been developed to study the effects of secondary water radiolysis caused by dispersed radionuclides in a bentonite buffer surrounding a copper canister. The secondary radiolysis is the radiolysis caused by radionuclides that have been released from the spent fuel and are present either as solutes in the pore-water, as sorbed species on the surface of other minerals, or as secondary minerals. The canister is assumed to be initially defective with a hole of a few millimeters on its wall. The small hole will considerably restrict the transport of oxidants through the canister wall and the release of radionuclides to the outside of the canister. The dissolution of the spent fuel is assumed to be controlled by chemical kinetics at rates extrapolated from experimental studies. Two cases have been considered with the purpose to illustrate the behaviors of both conservative and non-conservative nuclides. The nuclides that are most relevant are those expected to be the dominant α-emitters in the long-term (e.g. 239Pu, 240Pu, 241Am). In the first case it is assumed that there is no precipitation of secondary minerals of the relevant radionuclides inside the canister. In the second case it is assumed that the radionuclide concentration within the canister is controlled by its respective solubility limit. The radionuclide released to the surrounding buffer is then predicted using a mass balance model. The modelling results show that in both cases, the spent fuel will not be oxidized at a rate significantly faster compared to the case where secondary radiolysis is completely neglected. In the first case, however, a large domain of the near-field can be oxidized due to a much faster depletion of reducing minerals in the buffer, compared to the case where secondary radiolysis is neglected. In the second case, the effects of the secondary water radiolysis will be quite limited.

Processes Controlling Radionuclide Release from Spent Fuel

1994 ◽  
Vol 353 ◽  
Author(s):  
A. Loida ◽  
B. Grambow ◽  
H. Geckeis ◽  
P. Dressler
Keyword(s):  
Volume Ratio ◽  
Reaction Rates ◽  
Geometric Constraints ◽  
Spent Fuel ◽  
Oxidative Dissolution ◽  
Strong Decrease ◽  
Radiolysis Products ◽  
Upper Limits ◽  
Fuel Behavior ◽  
Radionuclide Release

AbstractDissolution of spent fuel has been studied in saline, anaerobe, carbonate free solutions. Processes controlling spent fuel dissolution and associated radionuclide release are radiolytically controlled oxidative dissolution, sorption on container, solubility and coprecipitation. Upper limits for oxidative dissolution rates are given by the production rates of oxidative radiolysis products. This limitation leads to a strong decrease in surface area normalized reaction rates with increasing surface to volume ratio (S/V) and imposes geometric constraints on prediction of spent fuel behavior in a repository. Solution concentrations of Am during spent fuel corrosion were about 5 orders of magnitude lower than the solubility of Am(OH)3(s) and are likely controlled by coprecipitation. Pu concentrations may be controlled by Pu(VI) or Pu(IV) (hydr)oxides.

Enhancement of Zirconolite Dissolution Due to Water Radiolysis

2006 ◽  
Vol 985 ◽  
Author(s):  
Nelly Toulhoat ◽  
Nelly Toulhoat ◽  
Nathalie Moncoffre ◽  
Pierre Toulhoat ◽  
Christophe Jegou ◽  
...  
Keyword(s):  
Charged Particle ◽  
Surface Water ◽  
Pure Water ◽  
Water Radiolysis ◽  
Water Interface ◽  
Spent Fuel ◽  
Enhanced Dissolution ◽  
Order Of Magnitude ◽  
Spent Fuel Reprocessing ◽  
Fuel Reprocessing

AbstractZirconolite is a candidate host material for conditioning minor tri- and tetra-valent actinides arising from enhanced nuclear spent fuel reprocessing and partitioning, in the case of disposal of the nuclear waste. Its chemical durability has been studied here under charged particle-induced radiolysis (He2+ and proton external beams) to identify the possible effects of water radiolysis on the dissolution rates in pure water and to describe the alteration mechanisms. Two experimental geometries have been used in order to evaluate the influence of the following parameters: solid irradiation, water radiolysis. In the first geometry the beam gets through the sample before stopping at the surface/water interface. In the second one the beam stops before the surface/water interface. Results on the elemental releases due to the enhanced dissolution of the zirconolite surface during charged particle-induced irradiation of water are presented. Under radiolysis, an increase of one order of magnitude is observed in the Ti, Zr and Nd elemental releases. No difference in the total elemental releases can be noticed when the solid is also irradiated.

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