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.

The Effect of Nearfield Constraints on the Corrosion Behavior of High Burnup Spent Fuel

2006 ◽  
Vol 932 ◽  
Author(s):  
Andreas Loida ◽  
Manfred Kelm ◽  
Bernhard Kienzler ◽  
Horst Geckeis ◽  
Andreas Bauer
Keyword(s):  
Host Rock ◽  
Near Field ◽  
Experimental Studies ◽  
Spent Fuel ◽  
Mutual Support ◽  
Significant Extent ◽  
Dissolution Rates ◽  
The Matrix ◽  
Container Material

ABSTRACTThe long-term immobilization for individual radioelements released from the waste form “spent fuel” in solid phases upon groundwater contact depends strongly on the (geo)chemical constraints prevailing in the repository. Related experimental studies comprise effects induced by the presence of Fe based container material, and near field materials other than Fe for a rock salt environment. The effect of the presence of an argillaceous host rock containing organic matter and pyrite on fuel alteration was studied in addition. The results have shown that oxidative radio-lysis products were found to be consumed at a significant extent by the metallic Fe and by the argillaceous host rock. Under these conditions a decrease at a factor of ca.100 for both the matrix dissolution rates and the solution concentrations of U and Pu was found. There is mutual support between the matrix dissolution rates, the solution concentrations and the amounts of oxygen encountered during the experiments under various conditions controlled by the presence of near field materials under study.

The geological research in France - The Dosssier 2005 Argile

2006 ◽  
Vol 985 ◽  
Author(s):  
Frederic Plas ◽  
Jacques WENDLING
Keyword(s):  
Near Field ◽  
Concept Design ◽  
Dose Calculations ◽  
Spent Fuel ◽  
Geological Medium ◽  
Source Data ◽  
Underground Research Laboratory ◽  
Broad Outline ◽  
Geological Research

AbstractAt the end of fifteen years of researchs defined by the French act of December 30, 1991 on radwaste management, Andra gave a report, “Dossier Argile 2005”, which concluded with the feasibility of a reversible disposal in the argillaceous Callovo-Oxfordien formation studied by means of an underground research laboratory at Meuse/Haute-Marne site. Starting from source data like the characteristics of the geological medium and the waste inventory, the process followed by Andra to achieve at this conclusion is of type sequential and iterative between concept design, scientific knowledge, in particular that of the phenomenological evolution of the reposiroty and its geological environment from operating period to long term, and Safety assessment. The “Dossier Argile 2005” covers a broad radwaste inventory, ILLW, HLW and Spent Fuel, so that it makes it possible to cover whole of the technological, scientific and safety topics. This article will give an overview of the geological disposal studies in France and draw the main conclusion of the Dossier 2005 Argile. It will be focused on the near field (Engineering components and near field host rock), while considering if necessary its integration within the whole system. After a short description of the concepts (incl. waste inventory and the characteristics of the Meuse/Haute the Marne site) and the functions of the components of repository and geological medium, one will describe successively the broad outline of the phenomenological evolution of repository and the geological medium in near field, by in particular releasing the time scales of processes and uncertainties of knowledge. On this basis, one will indicate the safety scenarios which were considered and the broad outline of performance and dose calculations. Lessons learn from the Dossier 2005 Argile will be discussed and perspective and priority for future will be indicated.

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.

Na/Ca selectivity coefficients of montmorillonite in perchlorate solution at different temperatures

2012 ◽  
Vol 1475 ◽  
Author(s):  
Aku Itälä ◽  
Arto Muurinen
Keyword(s):  
Cation Exchange ◽  
Spent Nuclear Fuel ◽  
Spent Fuel ◽  
Selectivity Coefficients ◽  
Crystalline Bedrock ◽  
Bentonite Buffer ◽  
Different Temperatures ◽  
C 50 ◽  
Exchange Selectivity

ABSTRACTThe Finnish spent nuclear fuel disposal is based on the Swedish KBS-3 concept in crystalline bedrock. The concept aims at long-term isolation and containment of spent fuel in copper canisters surrounded by bentonite buffer which mostly consists of montmorillonite. For the long-term modelling of the chemical processes in the buffer, the cation-exchange selectivity coefficients have to be known at different temperatures. In this work, the cation-exchange selectivity coefficients and cation-exchange isotherms were determined in batch experiments for montmorillonite at three different temperatures (25 °C, 50 °C and 75 °C). Five different ratios of NaClO4/Ca(ClO4)2 were used in the experimental solutions. After equilibration the solution and montmorillonite were separated and the solution analysed to get the desired exchange parameters. The experiments were modelled with a computational model capable of taking into account the physicochemical processes that take place in the experiment.

The Solubility and Sorption of Lead-210 and Carbon-14 in a Near-Field Environment

1987 ◽  
Vol 112 ◽  
Author(s):  
S. Bayliss ◽  
F. T. Ewart ◽  
R. M. Howse ◽  
J. L. Smith-Briggs ◽  
H. P. Thomason ◽  
...  
Keyword(s):  
Phase Separation ◽  
Near Field ◽  
Experimental Studies ◽  
Solubility Limit ◽  
Maximum Solubility ◽  
Separation Techniques ◽  
Sorption Behaviour ◽  
High Ph ◽  
Carbon 14 ◽  
Lead 210

AbstractThis paper reports the results of some recent experimental studies of the solubility and sorption behaviour of lead-210 and carbon-14 under cementitious near-field conditions.These studies have shown that under these conditions carbon-14 will have a maximum solubility limit of 10−4 M and that the distribution ratio, RD, will increase with increasing carbon-14 concentrations from 10−9 to 10−7 M. Not all of the carbon in the cement is available for exchange with carbon in the pore water. Differences in values of RD are observed between the two cement grout types studied, SRPC and OPC/BFS. Lead has been shown to have a maximum solubility limit of about 10−3 M at high pH. Good agreement is obtained between these measurements and thermodynamic modelling using the PHREEQE code. No differences were observed between lead solubilities under reducing or oxidising conditions at high pH values using the same phase separation techniques. Lead is particularly sensitive to the phase separation techniques employed. A factor of up to 250 difference is observed between 25000 and 30000 molecular weight cut-off filters. The values of RD for lead increase with decreasing lead concentrations and the values of RD for 10−3 M solutions are observed to be 500 mlg−1 for SRPC and 1300 mlg−1 for OPC/BFS.

Effect of Calcium Silicate Hydrate Precipitates at Cementitious and Bentonite Material Interface on Long-Term Engineered Barrier System Performance in TRU Waste Disposal Facilities

2009 ◽  
Vol 1193 ◽  
Author(s):  
Susumu Kurosawa ◽  
Hiroyuki Sakamoto ◽  
Kiyofumi Nitta ◽  
Chiya Numako ◽  
Kazuko Haga ◽  
...  
Keyword(s):  
Numerical Model ◽  
Mass Transport ◽  
Calcium Silicate ◽  
Calcium Silicate Hydrate ◽  
Experimental Studies ◽  
Material Interface ◽  
Long Period ◽  
Bentonite Buffer ◽  
Engineered Barrier

AbstractChemical conditions and mass transport properties of engineered barrier systems in TRU waste facilities would change with time due to the interaction of cement/bentonite materials. (‘TRU waste’ is one of categories of the radioactive wastes and contains a significant amount of alpha-emitting transuranic nuclides. In some countries, these wastes are classified into the Intermediate Level Waste (ILW).) Previous numerical model analyses to assess the long-term performance of engineered barrier systems in TRU waste repositories predicted to form Calcium Silicate Hydrate (C-S-H) species at the interface between the cementitious and bentonite materials. If C-S-H precipitates in the bentonite side of the boundary, mass transport in the bentonite buffer decreases and mineralogical alterations are expected to be restricted for a long period. The evidence of C-S-H precipitation in the bentonite side, however, still has not been identified in the former experimental studies. To improve the reliability of numerical analyses, immersion experiments were performed using contact samples of cementitious and bentonite materials, and X-ray absorption fine structure (XAFS) analysis was carried out to detect C-S-H precipitation at the contacting interface. Precipitation of C-S-H was confirmed from the obtained XAFS spectra. This result is one of the evidences to show the validity of the current numerical model analyses, which suggests that the bentonite buffer performance as an engineered barrier would be kept over a long period.

The IAEA Coordinated Research Programme on the Performance of High-Level Waste Forms and Packages Under Repository Conditions

1992 ◽  
Vol 294 ◽  
Author(s):  
Vladimir S. Tsyplenkov
Keyword(s):  
Near Field ◽  
Research Programme ◽  
High Level Waste ◽  
Future Research ◽  
Spent Fuel ◽  
Waste Forms ◽  
Safety Assessments ◽  
High Level ◽  
Coordination Meeting

ABSTRACTThe IAEA initiated, in 1991, a Coordinated Research Programme (CRP), with the aim of promoting the exchange of information on the results obtained by different countries in the performance of high-level waste forms and waste packages under conditions relevant to final repository. These studies are being undertaken to obtain reliable data as input to safety assessments and environmental impact analyses, for final disposal purposes. The CRP includes studies on waste forms that are presently of interest worldwide: borosilicate glass, Synroc and spent fuel.Ten laboratories leading in investigation of high-level waste form performance have already joined the programme. The results of their studies and plans for future research were presented at the first Research Coordination Meeting, held in Karlsruhe, Germany, in November 1991. The technical contributions concentrated on effecting an understanding of dissolution mechanisms of waste forms under simulated repository conditions. A quantitative interpretation of the chemical processes in the near field is considered a prerequisite for long-term predictions and for the formulation of a "source term" for performance assessment studies.

Mobilization/Retention of Radionuclides during Corrosion of High Burnup Spent Fuel and Backfill Materials in Salt Brines

2002 ◽  
Vol 757 ◽  
Author(s):  
Andreas Loida ◽  
Bernhard Kienzler ◽  
Horst Geckeis
Keyword(s):  
Near Field ◽  
Waste Form ◽  
Spent Fuel ◽  
The Matrix ◽  
Backfill Materials ◽  
Salt Brine ◽  
Solid Phases ◽  
Long Term Behavior ◽  
The Impact

ABSTRACTWith respect to the assessment of the long-term behavior of the waste form spent fuel it is of high importance to study the fuel alteration in contact with groundwater and near field materials. The aim of this work is to evaluate the impact of candidate backfill materials hydroxylapatite and magnetite on the overall corrosion behavior of this waste form in salt brine; both materials are used in corrosion tests together with spent fuel. The instant releases and the matrix dissolution rates appear to be similar in presence and in absence of any backfill material under study. However, Am,Np,Pu,U and Sr are retained at different ratios on the hydroxylapatite, on the magnetite and on the fuel sample, indicating possibly the formation of different radionuclide containing new solid phases.

Functional Requirements and Performance Assessment: Application to the Case of Spent Fuel Disposal in Clay

2001 ◽  
Author(s):  
Jan Marivoet ◽  
Xavier Sillen ◽  
Peter De Preter
Keyword(s):  
Molecular Diffusion ◽  
Slow Release ◽  
Near Field ◽  
Functional Requirements ◽  
Spent Fuel ◽  
Systematic Analysis ◽  
Boom Clay ◽  
Safety Function ◽  
Clay Formation

Abstract Geological repository systems for the disposal of radioactive waste are based on a multi-barrier design. Individual barriers contribute in different ways to the overall long-term performance of the repository system, and furthermore, the contribution of each barrier can considerably change with time. In a systematic analysis of the functional requirements for achieving long-term safety a number of basic safety functions can be defined: physical confinement, retardation / slow release, dispersion / dilution and limited accessibility. In the case of the geological disposal of spent fuel in a clay formation a series of barriers are designed or chosen to contribute to the realisation of the basic safety functions. The physical confinement is realised by the watertight, high-integrity container, which prevents contact between groundwater and the confined radionuclides. In first instance the retardation / slow release function is realised by the slow dissolution of the waste matrix and by the limited solubility of many elements in the near field. However, the natural clay barrier provides the main contribution to this safety function. The migration of radionuclides through the Boom Clay is mainly due to molecular diffusion, which is an extremely slow process. Furthermore, many elements are strongly sorbed by the clay minerals what makes their migration even much slower. The dispersion / dilution function mainly occurs in the aquifer and the rivers draining the aquifer in the surroundings of the disposal system. Various performance indicators are used to quantify the contributions of each safety function and to explain the functioning of the repository system.

SR 97: Spent Fuel Alteration/Dissolution and the Influence of Near Field Hydrogen

2000 ◽  
Vol 663 ◽  
Author(s):  
Kastriot Spahiu ◽  
Patrik Sellin
Keyword(s):  
Uranium Dioxide ◽  
Safety Assessment ◽  
Spent Nuclear Fuel ◽  
Near Field ◽  
Limiting Factor ◽  
Water Radiolysis ◽  
Spent Fuel ◽  
Reducing Conditions ◽  
S Matrix ◽  
The Matrix

ABSTRACTA discussion of the evaluation of the source term in the SR 97 safety assessment of a deep repository for spent nuclear fuel is presented. Since the majority of the radionuclides are embedded in the uranium dioxide fuel matrix, they will be released only after the alteration/dissolution of the matrix. Therefore a description of the process of alteration/dissolution of the spent fuel matrix is needed in a safety assessment.Under normal repository conditions, i.e. reducing environment and neutral to alkaline pH, uranium dioxide has a very low solubility in water. If solubility is assumed to be the limiting factor, the dissolution of the fuel matrix will proceed very slowly due to the low water exchange in the defective canister. On this basis, a solubility-limited model for the release of the radionuclides from the fuel may be formulated.The reducing conditions can be upset by the radioactivity of the spent fuel, which generates oxidizing products through water radiolysis. This causes the oxidative alteration/dissolution of the UO2(s) matrix. A model for fuel matrix conversion resulting from radiolytic oxidative dissolution is discussed, as well as parameter variations and the associated uncertainties.In a repository the spent fuel will come in contact with groundwater after the copper canister has breached. Large amounts of hydrogen are then produced through the anoxic corrosion of the cast iron insert. Recent data on spent fuel leaching in presence of repository relevant hydrogen pressures and the implications on the actual and future spent fuel dissolution modeling will also be discussed.

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