Release of Radiotoxic Elements from High Burn-Up UO2 and MOX Fuel in a Repository

2000 ◽  
Vol 663 ◽  
Author(s):  
Jean-Paul Glatz ◽  
Paul Carbol ◽  
Joaquin Cobos-Sabaté ◽  
Thomas Gouder ◽  
Frédéric Miserque ◽  
...  

ABSTRACTIn a spent fuel repository the processes that govern the release of radionuclides are dissolution and transport in a possible groundwater flow. The cladding will be the last barrier before the water comes into contact with the fuel, namely with the outer rim of the pellet. Here the heterogeneity of the material due to the irradiation process is responsible for a complex release process. Fission products and minor actinides inventories are considerably higher at the pellet periphery as a result of increased epithermal neutron capture and of migration in the case of the volatile fission products.The present paper gives a review of experimental activities at the Institute for Transuranium Elements (ITU). Both single effects studies and integral tests are carried out to study the behavior of spent fuel under storage conditions.Leaching of irradiated UO2 (up to 50 GWd/tU) and MOX (up to 25 GWd/tU) fuel rods with preset cladding defects at 100°C under anoxic or reducing conditions should simulate the realistic case of groundwater coming into contact with a spent nuclear fuel repository. For all main radionuclides the release process can be described considering a two-step dissolution mechanism that includes the initial dissolution of an oxidized layer present on the fuel surface followed by a long-term oxidative matrix dissolution. By means of α-doped (238Pu) UO2 it could be demonstrated, that radiolysis has a significant influence on this dissolution. Especially high initial release rates were found for the volatile cesium and iodine for the reasons mentioned above.Besides the conventional leaching experiments electrochemical techniques are used to investigate for instance the complex corrosion behavior of the heterogeneous MOX fuel materials or the influence of α-radiolysis on spent fuel dissolution.In the integral tests mentioned above with large S/V values, reprecipitation of U is likely to happen. Therefore special dynamic test are conducted where this reprecipitation is prohibited and true U solubility can be determined.Thin layer of UO2 and (U,Pu)O2 doped with various fission products and minor actinides are prepared to study the influence of these elements on the matrix dissolution. When Cs is for instance co-deposited, the U oxidation state changes from U4+ to U6+ for the same O2 pressure possibly indicating a stable Cs uranate. This could be an indirect proof of the existence of such a species in irradiated fuel (e.g. at the grain boundaries).

2013 ◽  
Vol 2013 ◽  
pp. 1-11 ◽  
Author(s):  
A. Schwenk-Ferrero

Germany is phasing-out the utilization of nuclear energy until 2022. Currently, nine light water reactors of originally nineteen are still connected to the grid. All power plants generate high-level nuclear waste like spent uranium or mixed uranium-plutonium dioxide fuel which has to be properly managed. Moreover, vitrified high-level waste containing minor actinides, fission products, and traces of plutonium reprocessing loses produced by reprocessing facilities has to be disposed of. In the paper, the assessments of German spent fuel legacy (heavy metal content) and the nuclide composition of this inventory have been done. The methodology used applies advanced nuclear fuel cycle simulation techniques in order to reproduce the operation of the German nuclear power plants from 1969 till 2022. NFCSim code developed by LANL was adopted for this purpose. It was estimated that ~10,300 tonnes of unreprocessed nuclear spent fuel will be generated until the shut-down of the ultimate German reactor. This inventory will contain ~131 tonnes of plutonium, ~21 tonnes of minor actinides, and 440 tonnes of fission products. Apart from this, ca.215 tonnes of vitrified HLW will be present. As fission products and transuranium elements remain radioactive from 104to 106years, the characteristics of spent fuel legacy over this period are estimated, and their impacts on decay storage and final repository are discussed.


2008 ◽  
Vol 96 (4-5) ◽  
Author(s):  
Mike T. Harrison ◽  
Howard E. Simms ◽  
Angela Jackson ◽  
Robert G. Lewin

Spent nuclear fuel may be treated using molten salt electrochemical techniques to separate fission products and actinide metals. Salt waste arising from the electrorefining process contains alkali metals, alkaline-earth and rare earth fission products, along with residual actinides. The removal of fission product elements has been investigated using zeolite ion exchange and phosphate precipitation, which allow the salt electrolyte to be recycled back into the main electrorefining vessel. Recycling the salt minimizes the volume of high level waste (HLW) generated and yields the fission products in a form more amenable to immobilization in a final disposal matrix. Several sets of experiments have been completed, all of which have significant implications for the use of these techniques on an industrial scale, as well as their ability to clean up the salt, and potentially produce robust and durable waste forms.


2008 ◽  
Vol 1104 ◽  
Author(s):  
Claude Degueldre ◽  
Wolfgang Wiesenack

AbstractA plutonia stabilised zirconia doped with yttria and erbia has been selected as inert matrix fuel (IMF) at PSI. The results of experimental irradiation tests on yttria-stabilised zirconia doped with plutonia and erbia pellets in the Halden research reactor as well as a study of zirconia solubility are presented. Zirconia must be stabilised by yttria to form a solid solution such as MAz(Y,Er)yPuxZr1-yO2-ζ where minor actinides (MA) oxides are also soluble. (Er,Y,Pu,Zr)O2-ζ (with Pu containing 5% Am) was successfully prepared at PSI and irradiated in the Halden reactor. Emphasis is given on the zirconia-IMF properties under in-pile irradiation, on the fuel material centre temperatures and on the fission gas release. The retention of fission products in zirconia may be stronger at similar temperature, compared to UO2. The outstanding behaviour of plutonia-zirconia inert matrix fuel is compared to the classical (U,Pu)O2 fuels. The properties of the spent fuel pellets are presented focusing on the once through strategy. For this strategy, low solubility of the inert matrix is required for geological disposal. This parameter was studied in detail for a range of solutions corresponding to groundwater under near field conditions. Under these conditions the IMF solubility is about 109 times smaller than glass, several orders of magnitude lower than UO2 in oxidising conditions (Yucca Mountain) and comparable in reducing conditions, which makes the zirconia material very attractive for deep geological disposal. The behaviour of plutonia-zirconia inert matrix fuel is discussed within a burn and bury strategy.


2002 ◽  
Vol 757 ◽  
Author(s):  
Yngve Albinsson ◽  
Arvid Ödegaard-Jensen ◽  
Virginia M. Oversby ◽  
Lars O. Werme

ABSTRACTSweden plans to dispose of spent nuclear fuel in a deep geologic repository in granitic rock. The disposal conditions allow water to contact the canisters by diffusion through the surrounding bentonite clay layer. Corrosion of the canister iron insert will consume oxygen and provide actively reducing conditions in the fluid phase. Experiments with spent fuel have been done to determine the dissolution behavior of the fuel matrix and associated fission products and actinides under conditions ranging from inert atmosphere to reducing conditions in solutions. Data for U, Pu, Np, Cs, Sr, Tc, Mo, and Ru have been obtained for dissolution in a dilute NaHCO3 groundwater for 3 conditions: Ar atmosphere, H2 atmosphere, and H2 atmosphere with Fe(II) in solution. Solution concentrations forU, Pu, and Mo are all significantly lower for the conditions that include Fe(II) ions in the solutions together with H2 atmosphere, while concentrations of the other elements seem to be unaffected by the change of atmospheres or presence of Fe(II). Most of the material that initially dissolved from the fuel has reprecipitated back onto the fuel surface. Very little material was recovered from rinsing and acid stripping of the reaction vessels.


Author(s):  
Yu. Pokhitonov ◽  
V. Romanovski ◽  
P. Rance

The principal purpose of spent fuel reprocessing consists in the recovery of the uranium and plutonium and the separation of fission products so as to allow re-use of fissile and fertile isotopes and facilitate disposal of waste elements. Amongst the fission products present in spent nuclear fuel of Nuclear Power Plants (NPPs,) there are considerable quantities of platinum group metals (PGMs): ruthenium, rhodium and palladium. Given current predictions for nuclear power generation, it is predicted that the quantities of palladium to be accumulated by the middle of this century will be comparable with those of the natural sources, and the quantities of rhodium in spent nuclear fuel may even exceed those in natural sources. These facts allow one to consider spent nuclear fuel generated by NPPs as a potential source for creation of a strategic stock of platinum group metals. Despite of a rather strong prediction of growth of palladium consumption, demand for “reactor” palladium in industry should not be expected because it contains a long-lived radioactive isotope 107Pd (half-life 6,5·105 years) and will thus be radioactive for a very considerable period, which, naturally, restricts its possible applications. It is presently difficult to predict all the areas for potential use of “reactor” palladium in the future, but one can envisage that the use of palladium in radwaste reprocessing technology (e.g. immobilization of iodine-129 and trans-plutonium elements) and in the hydrogen energy cycle may play a decisive role in developing the demand for this metal. Realization of platinum metals recovery operation before HLW vitrification will also have one further benefit, namely to simplify the vitrification process, because platinum group metals may in certain circumstances have adverse effects on the vitrification process. The paper will report data on platinum metals (PGM) distribution in spent fuel reprocessing products and the different alternatives of palladium separation flowsheets from HLW are presented. It is shown, that spent fuel dissolution conditions can affect the palladium distribution between solution and insoluble precipitates. The most important factors, which determine the composition and the yield of residues resulting from fuel dissolution, are the temperature and acid concentration. Apparently, a careful selection of fuel dissolution process parameters would make it possible to direct the main part of palladium to the 1st cycle raffinate together with the other fission products. In the authors’ opinion, the development of an efficient technology for palladium recovery requires the conception of a suitable flow-sheet and the choice of optimal regimes of “reactor” palladium recovery concurrently with the resolution of the problem of HLW partitioning when using the same facilities.


Author(s):  
Shengli Chen ◽  
Cenxi Yuan ◽  
Jingxia Wu ◽  
Yaolei Zou

The management of long-lived radionuclides in spent fuel is a key issue to achieve the closed nuclear fuel cycle and the sustainable development of nuclear energy. Partitioning-Transmutation is supposed to treat efficiently the long-lived radionuclides. Accordingly, the study of transmutation for long-lived Minor Actinides (MAs) is a significant work for the post-processing of spent fuel. In the present work, the transmutations in Pressurized Water Reactor (PWR) Mixed OXide (MOX) fuel are investigated through the Monte Carlo based code RMC. Two kinds of MAs are incorporated homogeneously into two initial concentrations MOX fuel assembly. The results indicate an overall nice efficiency of transmutation in both initial MOX concentrations, especially for two MAs primarily generated in the UOX fuel, 237Np and 241Am. In addition, the inclusion of 237Np has no large influence on other MAs, while the transmutation efficiency of 237Np is excellent. The transmutation of MAs in MOX fuel depletion is expected to be an efficient nuclear spent fuel management method.


2021 ◽  
Vol 13 (3) ◽  
pp. 41
Author(s):  
Р.М. Яковлев ◽  
И.А. Обухова

Large-scale nuclear energetics can satisfy demands for all kinds of energy, i.e. it can secure energy safety of Russia and the whole humankind; however, this is associated with a number of daunting problems. With that, this approach is a priority for Russia. The State Corporation RosAtom is involved in the development of nuclear reactors in Russia and abroad on the conditions that the reactors will be supplied with nuclear fuel from Russia and the spent fuel will be returned to Russia for conversion into mixed uranium and plutonium oxide (MOX) fuel. In the city Zheleznogorsk near Krasnoyarsk, the first production line of a plant for treating 2000 tons of spent nuclear fuel annually has been already launched. The principal strategic plan of RosAtom, which has been being realized currently, is to develop nuclear power production based on fuel recycling using fast neutron reactors for generation of plutonium, which may be used in nuclear weapons and is most hazardous for the biosphere. The possibility of accidents associated with radioactive discharges cannot be excluded, and the hazardousness of such accidents in increased by using plutonium-based fuels. The nuclear power-based approach to energy production is costly but also dangerous not only for Russia.


2019 ◽  
Vol 5 (3) ◽  
pp. 265-271 ◽  
Author(s):  
Andrey Yu. Petrov ◽  
Alexander V. Shutikov ◽  
Nikolay N. Ponomarev-Stepnoy ◽  
Valery S. Bezzubtsev ◽  
Mikhail V. Bakanov ◽  
...  

Possible options of organization of two-component energy system with closed nuclear fuel cycle (CNFC) and new business potential associated with provision of CFC services to foreign customers are examined. Dominating role in the development of nuclear power generation is assigned to VVER reactors with gradually increasing fraction of sodium-cooled fast breeder reactors (FR) incorporated within the joint nuclear fuel cycle operated on MOX-fuel. Components of such energy system perform the following functions: 1. Fast reactors: Generate electric power in base-load mode (possibility of fine tuning of reactor power within limited range (100 – 75 – 100%) is assumed); Utilize waste and/or regenerated uranium for re-fueling power reactors, produce plutonium applicable to the maximum extent for manufacturing MOX-fuel for VVER reactors; Incinerate long-lived highly radioactive wastes – minor actinides separated during reprocessing spent nuclear fuel of FR and VVER reactors. 2. VVER reactors: Generate electricity in compliance with manoeuvrability requirements imposed by the utility company operating the energy system; Utilize MOX-fuel instead of UO2 fuel; Are offered for export with the option of returning SNF back to Russia; Plutonium extracted from VVER spent fuel is used for manufacturing MOX-fuel for SFR. 3. Nuclear fuel cycle facilities: Provide reprocessing of SNF from VVER and SFR with extraction of nuclear materials for recycling; Use depleted or reprocessed uranium and plutonium extracted from spent nuclear fuel for manufacturing MOX-fuel; Provide partitioning of RAW for subsequent utilization of minor actinides and reduction of risks of proliferation of nuclear materials, conditioning and disposal of RAW. Russia possesses capacities for establishing the two-component system with CNFC, as well as the new business approach to rendering CNFC services to foreign customers.


2019 ◽  
Vol 322 (3) ◽  
pp. 1857-1862 ◽  
Author(s):  
Mu Lin ◽  
Ivan Kajan ◽  
Dorothea Schumann ◽  
Andreas Türler

Abstract During previous radioanalytical studies at Paul Scherrer Institute ca. 30 L of acidic waste containing spent nuclear fuel was produced, and now they need to be disposed A flow sheet for conditioning of these waste was designed and the extraction chromatography technique is evaluated. Suitable sorbents, such as AMP_PAN, TBP impregnated resin and DGA resin, were selected for the task of Cs-removal, extraction of U and Pu, and extraction of minor actinides and lanthanides, respectively. A pilot device will be built for preliminary tests with simulated solutions, and the facility will be built and evaluated with the real spent fuel solutions.


2019 ◽  
Vol 11 (22) ◽  
pp. 6364
Author(s):  
Sanggil Park ◽  
Min Bum Park

The OECD/NEA Spent Fuel Pool (SFP) project was conducted to investigate consequences of spent nuclear fuel pool accident scenarios. From the project, it was observed that cladding temperature could abruptly increase at a certain point and the cladding was completely oxidized. This phenomenon was called a “zirconium fire”. This zirconium fire is one of the crucial concerns for spent fuel pool safety under a postulated loss of coolant accident scenario, since it would lead to an uncontrolled mass release of fission products into the environment. To capture this critical phenomenon, an air-oxidation breakaway model has been implemented in the MELCOR code. This study examines this air-oxidation breakaway model by comparing the SFP project test data with a series of MELCOR code sensitivity calculation results. The air-oxidation model parameters are slightly altered to investigate their sensitivities on the occurrence of the zirconium fire. Through such sensitivity analysis, limitations of the air-oxidation breakaway model are identified, and needs for model improvement is recommended.


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