Leaching of Spent Fuel under Anaerobic and Reducing Conditions

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.

MRS Bulletin ◽  
1994 ◽  
Vol 19 (12) ◽  
pp. 24-27 ◽  
Author(s):  
L.H. Johnson ◽  
L.O. Werme

The geologic disposal of spent nuclear fuel is currently under consideration in many countries. Most of this fuel is in the form of assemblies of zirconium-alloy-clad rods containing enriched (1–4% 235U) or natural (0.71% 235U) uranium oxide pellets. Approximately 135,000 Mg are presently in temporary storage facilities throughout the world in nations with commercial nuclear power stations.Safe geologic disposal of nuclear waste could be achieved using a combination of a natural barrier (the host rock of the repository) and engineered barriers, which would include a low-solubility waste form, long-lived containers, and clay- and cement-based barriers surrounding the waste containers and sealing the excavations.A requirement in evaluating the safety of disposal of nuclear waste is a knowledge of the kinetics and mechanism of dissolution of the waste form in groundwater and the solubility of the waste form constituents. In the case of spent nuclear fuel, this means developing an understanding of fuel microstructure, its impact on release of contained fission products, and the dissolution behavior of spent fuel and of UO2, the principal constituent of the fuel.


2000 ◽  
Vol 6 (S2) ◽  
pp. 368-369
Author(s):  
N.L. Dietz ◽  
D.D Keiser

Argonne National Laboratory has developed an electrometallurgical treatment process for metallic spent nuclear fuel from the Experimental Breeder Reactor-II. This process stabilizes metallic sodium and separates usable uranium from fission products and transuranic elements that are contained in the fuel. The fission products and other waste constituents are placed into two waste forms: a ceramic waste form that contains the transuranic elements and active fission products such as Cs, Sr, I and the rare earth elements, and a metal alloy waste form composed primarily of stainless steel (SS), from claddings hulls and reactor hardware, and ∼15 wt.% Zr (from the U-Zr and U-Pu-Zr alloy fuels). The metal waste form (MWF) also contains noble metal fission products (Tc, Nb, Ru, Rh, Te, Ag, Pd, Mo) and minor amounts of actinides. Both waste forms are intended for eventual disposal in a geologic repository.


Author(s):  
Krista Nicholson ◽  
John McDonald ◽  
Shona Draper ◽  
Brian M. Ikeda ◽  
Igor Pioro

Currently in Canada, spent fuel produced from Nuclear Power Plants (NPPs) is in the interim storage all across the country. It is Canada’s long-term strategy to have a national geologic repository for the disposal of spent nuclear fuel for CANada Deuterium Uranium (CANDU) reactors. The initial problem is to identify a means to centralize Canada’s spent nuclear fuel. The objective of this paper is to present a solution for the transportation issues that surround centralizing the waste. This paper reviews three major components of managing and the transporting of high-level nuclear waste: 1) site selection, 2) containment and 3) the proposed transportation method. The site has been selected based upon several factors including proximity to railways and highways. These factors play an important role in the site-selection process since the location must be accessible and ideally to be far from communities. For the containment of the spent fuel during transportation, a copper-shell container with a steel structural infrastructure was selected based on good thermal, structural, and corrosion resistance properties has been designed. Rail has been selected as the method of transporting the container due to both the potential to accommodate several containers at once and the extensive railway system in Canada.


Author(s):  
Jenny Morris ◽  
Stephen Wickham ◽  
Phil Richardson ◽  
Colin Rhodes ◽  
Mike Newland

The UK Nuclear Decommissioning Authority (NDA) is responsible for safe and secure management of spent nuclear fuel. Magnox spent fuel is held at some Magnox reactor sites and at Sellafield where it is reprocessed using a number of facilities. It is intended that all Magnox fuel will be reprocessed, as described in the published Magnox Operating Plan (MOP) [1]. In the event, however, that a failure occurs within the reprocessing plant, the NDA has initiated a programme of activities to explore alternative contingency options for the management of wetted Magnox spent fuel. Magnox fuel comprises metallic uranium bar clad in a magnesium alloy, both of which corrode if exposed to oxygen or water. Consequently, contingency options are required to consider how best to manage the issues associated with the reactivity of the metals. Questions of whether Magnox spent fuel needs to be dried, how it might be conditioned, how it might be packaged, and held in temporary storage until a disposal facility becomes available, all require attention. A review of potential contingency options for Magnox fuel was conducted by Galson Sciences Ltd, UKAEA and the NDA. During storage in the presence of water, the corrosion of Magnox fuel produces hydrogen (H2) gas, which requires careful management. When uranium reacts with hydrogen in a reducing environment, the formation of uranium hydride (UH3) may occur, which under some circumstances can be pyrophoric, and might create hazards which may affect subsequent retrieval and/or repackaging (e.g. for disposal). Other factors that may affect the choice of a viable contingency option include criticality safety, environmental impacts, security and Safeguards and economic considerations. At post-irradiation examination (PIE) facilities in the UK, Magnox spent fuel is dried as a result of storage in air at ambient temperatures. Early French UNGG (Uranium Naturel Graphite Gaz) fuel was retrieved from pond storage at Cadarache, dried using a hot gas drying technique, oxidised and packaged in sealed canisters and placed in interim storage at the CASCAD (CASemate CADarache) facility. In the US, spent fuels including the Zircaloy clad Hanford N-Reactor fuels were cold vacuum dried and Idaho legacy aluminium clad metallic uranium fuels were hot vacuum dried; the dried fuel was then packaged in sealed and vented canisters (at Hanford and Idaho, respectively) for interim storage. With regard to conditioning and packaging, several different approaches have been reviewed, including encapsulation in cementitious grout or polymer, high-temperature vitrification or ceramicisation, and solution in acid or alkali solution followed by cementation or vitrification (without reprocessing). All of these approaches require further research in order to be evaluated and developed further for application to formerly wetted Magnox fuel. A variety of containers have been developed for the transport, storage and/or disposal of spent fuel in radioactive waste management programmes worldwide. Wetted Magnox spent fuel could be packaged in a container, with reservations about the potential formation of UH3 in a sealed environment where reducing conditions may develop. The applicability of different combinations of drying, conditioning and packaging techniques to the preparation of Magnox spent fuel for long-term storage and eventual disposal are discussed.


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.


1996 ◽  
Vol 465 ◽  
Author(s):  
C. W. Forsberg

ABSTRACTA new repository waste package (WP) concept for spent nuclear fuel (SNF) is being investigated. The WP uses depleted uranium (DU) to improve performance and reduce the uncertainties of geological disposal of SNF. The WP would be loaded with SNF. Void spaces would then be filled with DU (∼0.2 wt % 235U) dioxide (UO2) or DU silicate-glass beads.Fission products and actinides can not escape the SNF UO2 crystals until the UO2 dissolves or is transformed into other chemical species. After WP failure, the DU fill material slows dissolution by three mechanisms: (1) saturation of WP groundwater with DU and suppression of SNF dissolution, (2) maintenance of chemically reducing conditions in the WP that minimize SNF solubility by sacrificial oxidation of DU from the +4 valence state, and (3) evolution of DU to lower-density hydrated uranium silicates. The fill expansion minimizes water flow in the degraded WP. The DU also isotopically exchanges with SNF uranium as the SNF degrades to reduce long-term nuclear-criticality concerns.


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):  
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.


1989 ◽  
Vol 176 ◽  
Author(s):  
Y. Albinsson ◽  
R. Forsyth ◽  
G. Skarnemark ◽  
M. Skålberg ◽  
B. Torstenfelt ◽  
...  

ABSTRACTThe release and migration of the fission products cesium, europium and technetium, the actinides plutonium, americium and curium, and the activation product cobalt from spent nuclear fuel pellets in highly compacted bentonite clay has been measured after contact times of 101 and 386 days. Experiments at longer contact times are in progress. In some cases small amounts (0.5–1%) of powdered copper or iron metal, or vivianite (Fe3(PO4)2) have been mixed with the bentonite clay.The results indicate as expected a high mobility of cesium. The actinides have a very low mobility. After 386 days, plutonium has diffused less than 0.5 mm away from the fuel, while americium and curium appear to be somewhat more mobile. The behaviour of europium is similar to that of trivalent actinides. Very little technetium has been leached from all samples. Cobalt shows a strong retention in pure bentonite as well as in the presence of vivianite, while the mobility is much larger when iron or copper is added.


2002 ◽  
Vol 90 (9-11) ◽  
Author(s):  
S. Stroes-Gascoyne ◽  
F. King ◽  
J. S. Betteridge ◽  
F. Garisto

SummaryThe long-term stability of spent nuclear fuel under deep geologic repository conditions will be determined mostly by the influence of α-radiolysis, since the dose-rate for α-radiolysis will exceed that for γ/β-radiolysis beyond a fuel age of ∼100 years and will persist for more than 10000 years. Dissolution rates derived from studies with currently available spent fuel include radiolysis effects from γ/β- as well as α-radiolysis. The use of external α-sources and chemically added H


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