A New Approach to the RN Source Term for Spent Nuclear Fuel under Geological Disposal Conditions

2000 ◽  
Vol 663 ◽  
Author(s):  
Christophe Poinssot ◽  
Christophe Jegou ◽  
Pierre Toulhoat ◽  
Jean-Paul Piron ◽  
Jean-Marie Gras

ABSTRACTUnder the geological disposal conditions, spent fuel (SF) is expected to evolve during the 10,000 years while being maintained isolated from the biosphere before coming in contact with water. Under these circumstances, several driving forces would lead to the progressive intrinsic transformations within the rod which would modify the subsequent release of radionuclides. The major mechanisms are the production of a significant volume of He within the UO2 lattice, the accumulation of irradiation defects due to the low temperature which avoids any annealing, the slow migration of radionuclides (RN) within the system by (i) the α self-irradiation-induced athermal diffusion and (ii) locally the building-up of internal mechanical stresses which could turn the pellets into powder. However, the current RN source terms for SF have never accounted for this evolution as they are based on existing knowledge of 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 take account of the early evolution of the closed system, the amplitude of which increases with the burnup and is greater for MOX fuels.

Author(s):  
Christophe Poinssot ◽  
Christophe Jegou ◽  
Pierre Toulhoat ◽  
Jean-Marie Gras

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.


Author(s):  
Lara Duro ◽  
Abel Tamayo ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza

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.


Molecules ◽  
2020 ◽  
Vol 25 (6) ◽  
pp. 1429 ◽  
Author(s):  
Víctor Vicente Vilas ◽  
Sylvain Millet ◽  
Miguel Sandow ◽  
Luis Iglesias Pérez ◽  
Daniel Serrano-Purroy ◽  
...  

To reduce uncertainties in determining the source term and evolving condition of spent nuclear fuel is fundamental to the safety assessment. ß-emitting nuclides pose a challenging task for reliable, quantitative determination because both radiometric and mass spectrometric methodologies require prior chemical purification for the removal of interfering activity and isobars, respectively. A method for the determination of 90Sr at trace levels in nuclear spent fuel leachate samples without sophisticated and time-consuming procedures has been established. The analytical approach uses a commercially available automated pre-concentration device (SeaFAST) coupled to an ICP-DRC-MS. The method shows good performances with regard to reproducibility, precision, and LOD reducing the total time of analysis for each sample to 12.5 min. The comparison between the developed method and the classical radiochemical method shows a good agreement when taking into account the associated uncertainties.


2002 ◽  
Vol 713 ◽  
Author(s):  
Christophe Poinssot ◽  
Patrick Lovera ◽  
Marie-Hélène Faure

ABSTRACTUnder the geological disposal conditions, spent nuclear fuel (SNF) is expected to evolve during the first thousands years while being maintained isolated from the biosphere before water comes in. Under those circumstances, several driving forces would lead to the progressive intrinsic SNF transformations within the rod which would basically modify the physical and chemical state of the fuel and the subsequent release of radionuclides in solution. In this paper, we briefly summarize the mechanisms we estimate to be significant and propose a new framework for the quantitative assessment of the radionuclide (RN) inventory we estimate to be associated to the classically referred to “Instant Release Fraction” (IRF). We hence demonstrate that in this framework, significantly high IRF values have to be expected for the long term due mainly to the presence of athermal diffusion processes.


2020 ◽  
Vol 6 (2) ◽  
pp. 93-98
Author(s):  
Nikita V. Kovalev ◽  
Boris Ya. Zilberman ◽  
Nikolay D. Goletsky ◽  
Andrey B. Sinyukhin

A review of simulated nuclear fuel cycles with mixed uranium-plutonium fuel (REMIX) was carried out. The concept of REMIX fuel is one of the options for closing the nuclear fuel cycle (NFC), which makes it possible to recycle uranium and plutonium in VVER-1000/1200 thermal reactors at a 100% core loading. The authors propose a new approach to the recycling of spent nuclear fuel (SNF) in thermal reactors. The approach implies a simplified fabrication of mixed fuel when plutonium is used in high concentration together with enriched natural uranium, while reprocessed uranium is supposed to be enriched and used separately. The share of standard enriched natural uranium fuel in this nuclear fuel cycle is more than 50%, the share of mixed natU+Pu fuel is 25%, the rest is fuel obtained from enriched reprocessed uranium. It is emphasized that the new approach has the maximum economic prospect and makes it possible to organize the fabrication of this fuel and nuclear material cross-cycling at the facilities available in the Russian Federation in the short term. This NFC option eliminates the accumulation of SNF in the form of spent fuel assemblies (SFA). SNF is always reprocessed with the aim of further using the primary reprocessed uranium and plutonium. Non-recyclable in thermal reactors, burnt, reprocessed uranium, the energy potential of which is comparable to natural uranium, as well as secondary plutonium intended for further use in fast reactors, are sent as reprocessing by-products to the storage area.


2015 ◽  
Vol 1744 ◽  
pp. 217-222
Author(s):  
O. Roth ◽  
M. Granfors ◽  
A. Puranen ◽  
K. Spahiu

ABSTRACTIn a future Swedish deep repository for spent nuclear fuel, irradiated control rods from PWR nuclear reactors are planned to be stored together with the spent fuel. The control rod absorber consists of an 80% Ag, 5% Cd, 15% In alloy with a steel cladding. Upon in-reactor irradiation 108Ag is produced by neutron capture. Release of 108Ag has been identified as a potential source term for release of radioactive substances from the deep repository.Under reducing deep repository conditions, the Ag corrosion rate is however expected to be low which would imply that the release rate of 108Ag should be low under these conditions. The aim of this study is to investigate the dissolution of PWR control rod absorber material under conditions relevant to a future deep repository for spent nuclear fuel. The experiments include tests using irradiated control rod absorber material from Ringhals 2, Sweden. Furthermore, un-irradiated control rod absorber alloy has been tested for comparison. The experiments indicate that the release of Ag from the alloy when exposed to water is strongly dependent on the redox conditions. Under aerated conditions Ag is released at a significant rate whereas no release could be measured after 133 days during leaching under H2.


2004 ◽  
Vol 824 ◽  
Author(s):  
Christophe Poinssot ◽  
Patrick Lovera ◽  
Cécile Ferry

AbstractIn the framework of the research conducted on the long term evolution of spent nuclear fuel in geological disposal conditions, a source term model has been developed to evaluate the instantaneous release of RN (Instant Release Fraction IRF) and the delayed release of the RN which are embedded within the matrix. This model takes into account all the scientific results currently available in the literature except the hydrogen effect. IRF was assessed by considering the evolution with time of the RN inventories located within the fuel microstructure to which no confinement properties can be allocated on the long term (rim, gap, grain boundaries). It allows to propose some reference bounding values for the IRF as a function of time of canister breaching and burnup. The matrix radiolytic dissolution was modeled by a simple kinetic model neglecting the radiolytic species recombination and the influence of aqueous ligands and radiolytic oxidants were supposed to completely react with the fuel surface. Spent fuel performance was therefore demonstrated to deeply depend on the reactive surface area.


Author(s):  
Sergey Yu. Sayenko ◽  
G. A. Kholomeyev ◽  
B. A. Shilyaev ◽  
A. V. Pilipenko ◽  
E. P. Shevyakova ◽  
...  

Abstract This paper describes the research work carried out at the NSC KIPT to develop and apply a final waste form in the shape of a monolithic solid block for the containment of spent nuclear fuel. To prepare radioactive waste for long-term storage and final deep geological disposal, investigations into the development of methods of immobilizing HLW simulators in protective solid matrices are being conducted at the NSC KIPT. For RBMK spent nuclear fuel it is proposed and justified to encapsulate the spent fuel bundles into monolithic protective blocks, produced with the help of hot isostatic pressing (HIP) of powder materials. In accordance with this approach, as a material for the protective block made up of the glass-ceramic composition prepared by sintering at isostatic pressure, the powder mixture of such natural rocks as granite and clay has been chosen. Concept approach and characterization of waste form, technological operations of manufacturing and performance assessment are presented. The container with spent fuel for long-term storage and final disposal presents a three barrier protective system: ceramic fuel UO2 in cladding tube, material of the glass-ceramic block, material of the sealed metal capsule. Investigations showed that the produced glass-ceramic material is characterized by high stability of chemical and phase compositions, high resistance in water medium, low porosity (compared with the porosity of natural basalt). With the help of mathematical calculations it was shown that the absorbed dose of immobilizing material by RBMK spent fuel irradiation for 1000 years of storage in the geological disposal after 10 years of preliminary cooling will be ∼ 3.108 Gy, that is 2–3 orders of magnitude less than the values corresponding to preserving radiation resistance and functional parameters of glasses and ceramics. The average value of velocity of linear corrosion in water medium of the protective layer made up of the glass-ceramic composition determined experimentally makes up ∼ 15 mm per year. This allows to use glass-ceramic compositions effectively as an engineering barrier in the system of spent fuel geological disposal and to increase the lifetime of the waste container, in particular, up to 3000 years with the layer thickness ∼ 40 mm. The possible release of radionuclides from the waste container during its interim storage in the open air (near-surface storage) is estimated. The calculations are made by taking into account the possible increase of coefficients of radionuclide diffusion from 10−16 to 10−14 m2/c as a result of spent fuel radiation affecting the protective layer. The obtained results showed that the protective barrier (about 40 mm) at the base of the glass-ceramic composition, ensures reliable isolation from the environment against the release of radionuclides from the controlled near-surface long-term storage far up to 1000 years. The relatively limited release of radionuclides will make up about 1% for the period of more than 400 years, and 10% - in 1000 years. During this period of time, the radionuclides 90Sr and 137Cs will completely turn into stable 90Zr and 137Ba and the decay of many transuranium elements will occur. The results from laboratory scale experiments, tests and calculations carried out so far, show that the proposed glass-ceramic materials may be used as basic materials for manufacturing the monolithic protective block in which the spent fuel elements will be embedded with the aim of further long-term storage or final disposal.


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