α-Radiolysis and α-Radiation Damage Effects on uo2 Dissolution Under Spent Fuel Storage Conditions

1999 ◽  
Vol 556 ◽  
Author(s):  
V. V. Rondinella ◽  
Hj. matzke ◽  
J. Cobos ◽  
T. Wiss

Abstractα-decay will constitute almost entirely the radiation field in and around spent nuclear fuel after a few hundred years in a geological repository. Pellets of UO 2 containing ˜0.1 and ˜10 wt. % 238Pu were fabricated using a sol-gel method and characterized, comparing their properties to those of undoped UO2. The α-radiation fields of different types of commercial LWR spent fuel are of the same order of magnitude as the fuel with the lower Pu-concentration used in this work. The results of static batch leaching tests at room temperature in demineralized water under anoxic atmosphere showed that the amounts of U released during leaching were higher in the case of UO2 containing 238pu than for undoped UO2. Relatively large amounts of Pu were released after the longest leaching times. Lattice parameter measurements using XRD and hardness measurements by Vickers indentation showed a relatively rapid build-up of α-decay damage in the material stored at ambient temperature with the higher concentration of dopant, while for the material with ˜0.1 wt. % Pu no clear variations were detected during the same time intervals.

MRS Advances ◽  
2017 ◽  
Vol 2 (13) ◽  
pp. 711-716 ◽  
Author(s):  
Lovisa Bauhn ◽  
Christian Ekberg ◽  
Patrik Fors ◽  
Kastriot Spahiu

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.


Author(s):  
Donald Wayne Lewis

In the United States (U.S.) the nuclear waste issue has plagued the nuclear industry for decades. Originally, spent fuel was to be reprocessed but with the threat of nuclear proliferation, spent fuel reprocessing has been eliminated, at least for now. In 1983, the Nuclear Waste Policy Act of 1982 [1] was established, authorizing development of one or more spent fuel and high-level nuclear waste geological repositories and a consolidated national storage facility, called a “Monitored Retrievable Storage” facility, that could store the spent nuclear fuel until it could be placed into the geological repository. Plans were under way to build a geological repository, Yucca Mountain, but with the decision by President Obama to terminate the development of Yucca Mountain, a consolidated national storage facility that can store spent fuel for an interim period until a new repository is established has become very important. Since reactor sites have not been able to wait for the government to come up with a storage or disposal location, spent fuel remains in wet or dry storage at each nuclear plant. The purpose of this paper is to present a concept developed to address the DOE’s goals stated above. This concept was developed over the past few months by collaboration between the DOE and industry experts that have experience in designing spent nuclear fuel facilities. The paper examines the current spent fuel storage conditions at shutdown reactor sites, operating reactor sites, and the type of storage systems (transportable versus non-transportable, welded or bolted). The concept lays out the basis for a pilot storage facility to house spent fuel from shutdown reactor sites and then how the pilot facility can be enlarged to a larger full scale consolidated interim storage facility.


2004 ◽  
Vol 824 ◽  
Author(s):  
Danièle Roudil ◽  
Xavier Deschanels ◽  
Patrick Trocellier ◽  
Fran ç ois Jomard ◽  
Annick Boutry ◽  
...  

AbstractThe behaviour and diffusion mechanisms of helium in nuclear ceramics, such as uranium dioxide spent fuel matrix and zirconolite for the specific conditioning of minor actinides, significantly impact the possible evolution of those matrices in interim storage or disposal conditions. In the framework of spent fuel storage studies, the additional diffusion of gas and fission products in uranium dioxidematrix is also an essential aspect of the R&D. Specific experimental studies have been conducted, devoted to thermal diffusion under 1000 C. Data processing methods, lead to helium diffusion coefficient and associated activation energy of 1.05 eV in the zirconolite and 2 eV in UO2. Comparativelywith the uranium dioxide matrix, the helium diffusion coefficient in zirconolite is 1 to 100 million times higher; this parameter will have to be taken into account to dimension the waste form. Diffusion coefficients measurements between 800 C and 1000 C, investigated by SIMS, showed a very slow diffusion of volatile fission products Xe, I, Te and Cs, with coefficients two or three order of magnitude lower than for helium.


MRS Advances ◽  
2016 ◽  
Vol 1 (62) ◽  
pp. 4147-4156 ◽  
Author(s):  
C. Ferry ◽  
J. Radwan ◽  
H. Palancher

ABSTRACTHelium is produced in spent nuclear fuel by α-decays of actinides. After 10,000 years, the concentration of He accumulated in UO2 spent fuel is about 0.23 at.%. For direct disposal of spent nuclear fuel, consequences of helium build-up on the fuel matrix microstructure must be evaluated since it can modify the radionuclide release when water comes into contact with the spent fuel surface, after breaching of the disposal canister. An operational model has been proposed in order to evaluate the effect of helium on the microstructure of spent fuel in a repository. Based on conservative assumptions and different scenarios of bubble population, the calculated helium critical concentration, that could lead to a partial loss of integrity of the spent fuel pellet, is 0.37 at.%. However, observations on He-implanted UO2, α-doped UO2 pellets and natural analogues evidence a macroscopic damage only for He concentrations, which are more than one order of magnitude higher.


2019 ◽  
pp. 82-87
Author(s):  
Ya. Kostiushko ◽  
O. Dudka ◽  
Yu. Kovbasenko ◽  
A. Shepitchak

The introduction of new fuel for nuclear power plants in Ukraine is related to obtaining a relevant license from the regulatory authority for nuclear and radiation safety of Ukraine. The same approach is used for spent nuclear fuel (SNF) management system. The dry spent fuel storage facility (DSFSF) is the first nuclear facility created for intermediate dry storage of SNF in Ukraine. According to the design based on dry ventilated container storage technology by Sierra Nuclear Corporation and Duke Engineering and Services, ventilated storage containers (VSC-VVER) filled with SNF of VVER-1000 are used, which are located on a special open concrete site. Containers VSC-VVER are modernized VSC-24 containers customized for hexagonal VVER-1000 spent fuel assemblies. The storage safety assessment methodology was created and improved directly during the licensing process. In addition, in accordance with the Energy Strategy of Ukraine up to 2035, one of the key task is the further diversification of nuclear fuel suppliers. Within the framework of the Executive Agreement between the Government of Ukraine and the U.S. Government, activities have been underway since 2000 on the introduction of Westinghouse fuel. The purpose of this project is to develop, supply and qualify alternative nuclear fuel compatible with fuel produced in Russia for Ukrainian NPPs. In addition, a supplementary approach to safety analysis report is being developed to justify feasibility of loading new fuel into the DSFSF containers. The stated results should demonstrate the fulfillment of design criteria under normal operating conditions, abnormal conditions and design-basis accidents of DSFSF components.  Thus, the paper highlights both the main problems of DSFSF licensing and obtaining permission for placing new fuel types in DSFSF.


Author(s):  
Earl Easton ◽  
Christopher Bajwa ◽  
Zhian Li ◽  
Matthew Gordon

The current uncertainty surrounding the licensing and eventual opening of a long term geologic repository for the nation’s civilian and defense spent nuclear fuel (SNF) and high level radioactive waste (HLW) has shifted the window for the length of time spent fuel could be stored to periods of time significantly longer than the current licensing period of 40 years for dry storage. An alternative approach may be needed to the licensing of high-burnup fuel for storage and transportation based on the assumption that spent fuel cladding may not always remain intact. The approach would permit spent fuel to be retrieved on a canister basis and could lessen the need for repackaging of spent fuel. This approach is being presented as a possible engineering solution to address the uncertainties and lack of data availability for cladding properties for high burnup fuel and extended storage time frames. The proposed approach does not involve relaxing current safety standards for criticality safety, containment, or permissible external dose rates.


Author(s):  
V. Zaiets

Zaporozhye Nuclear Power Plant (NPP) commissioned a Spent-Fuel Dry-Storage Facility (SFDSF) with a 50-year service life. The SFDSF design is based on the proven technology of the US Duke Engineering & Services Company and meets international standards, rules and regulations on nuclear and radiation safety [1]. The objectives of this paper are calculation of the external neutron and γ-radiation of a single container, and prediction of radiation characteristics during a storage period up to 50 years. The calculations were made for VSC-24 special ventilated containers manufactured by Sierra Nuclear Corporation (USA) [2]. The analysis shows that the change in gamma energy spectrum results in a faster decrease in dose with time which is in agreement with observations in the SFDSF. The γ-radiation dose rate is mainly composed of 0.5 to 2.5 MeV quanta.


2021 ◽  
Vol 11 (16) ◽  
pp. 7362
Author(s):  
Arturas Smaizys ◽  
Ernestas Narkunas ◽  
Gintautas Poskas ◽  
Povilas Poskas

The present SF management concept in Lithuania envisages that spent RBMK-1500 fuel will be stored in dry storage containers for 50 years, before being disposed of in a deep geological repository. However, the risk that a deep geological repository will not be constructed at the planned time should be taken into account, and the extension of SF storage over 50 years should be considered. This paper presents a comparison of gamma and neutron dose rate distributions and variations with planned and extended storage times for cast iron and metal–concrete containers loaded with RBMK-1500 SF. All calculations were performed using the SCALE computer codes system. The modeling results show that the overall shielding properties of the CONSTOR® RBMK-1500 container containing the same neutron and gamma sources are better than those of the CASTOR® RBMK-1500 container. During an extended storage period (from 50 to 300 years), the total dose rate would decrease considerably and the dose rate due to neutrons would become dominant for both containers.


2006 ◽  
Vol 932 ◽  
Author(s):  
Christophe Poinssot ◽  
Cécile Ferry ◽  
Bernd Grambow ◽  
Manfred Kelm ◽  
Kastriot Spahiu ◽  
...  

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.


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