Uraninite: a 2 Ga Spent Nuclear Fuel from the Natural Fission Reactor at Bangombé in Gabon, West Africa

1996 ◽  
Vol 465 ◽  
Author(s):  
K. A. Jensen ◽  
R. C. Ewing ◽  
F. Gauthier-Lafaye

ABSTRACTUraninites from the Bangombé natural fission reactor (RZB) and “normal” uranium-ore occur as fine veins in the sandstone host-rock as well as altered, broken, and slightly displaced grains in an illitic matrix, and in nodules and veins of solid bitumen. Inclusions of galena, (Y,Gd)-rich phosphates, a Pb-oxide and a Ti-oxide? were observed. Uraninites just below RZB were partially altered to a uranyl-sulfate. Three generations of uraninite were identified based on their PbO-contents of 8–11.06 wt%, 6 wt% (the largest population), and a younger generation with 3 wt%. The high Pb-uraninites may be the precursor to the low Pb-uraninites. Diffusional loss of Pb is indicated by the presence of a Pb-oxide at the interface to the uraninites. The behaviour of the metallic fission products, incompatible with the uraninite structure, may mimic the behaviour of Pb in these uraninites. The averaged impurity-content ranges from 4.29 to 6.89 wt%, and consists mainly of SiO2, TiO2, ZrO2, FeO, CaO, Al2O3 and P2O5. The averaged content of Y2O3 and the Ln's is less than 0.78 wt% and there is a scattered positive correlation with P2O5. The content of Y + Ln's is generally highest in the uraninites from RZB. Uraninite hydration and the formation of “uranopelite/zippeite” have caused complete loss of Y and the Ln's. These elements seems also to be partially lost by weak phosphatian coffinitization. The analytical results indicate that Y and the Ln's, which are high yield fission products, may be released from uraninite during alteration in the presence of P.

2020 ◽  
Vol 108 (8) ◽  
pp. 615-626
Author(s):  
Mu Lin ◽  
Ivan Kajan ◽  
Dorothea Schumann ◽  
Andreas Türler ◽  
Adelheid Fankhauser

AbstractThirty liters of highly acidic spent nuclear fuel solutions need to be disposed at the “Hot Laboratory (hotlab)” facility in Paul Scherrer Institut (PSI), Switzerland. In order to significantly reduce the γ dose rate before proper disposal treatment, 137Cs must be removed. In the here presented sub-project, the ion-exchange method was evaluated. Two promising sorbents, CLEVASOL® and AMP (ammonium molybdophosphate), and two derived products AMP_PAN (AMP immobilized in polyacrylonitrile) and AMP/SiO2 (AMP immobilized on silica gel) were tested by the batch method using model solutions of important high-yield fission products (Cs, Eu, Zr, Ru, Pd and Ag), as well as U and Pu. The results showed that AMP, AMP/SiO2 and AMP_PAN have higher selectivity for Cs than CLEVASOL® in 0.1–8 M (mol/L) HNO3 solutions. 4 M HNO3 solution was identified as the most suitable condition for Cs-removal with AMP, AMP_PAN and AMP/SiO2 due to the still sufficiently high separation factor of Cs from other metal ions and an acceptable volume increase factor after dilution. The follow-up kinetic studies on AMP, AMP_PAN and AMP/SiO2 indicated that although Cs exchange on AMP and AMP/SiO2 is faster than on AMP_PAN in the first 5 min, they all nearly reach equilibrium after 30 min of contacting time. The isotherm curves of Cs adsorption on AMP, AMP_PAN and AMP/SiO2 in 4 M HNO3 showed that the maximum sorption capacity of Cs is reached asymptotically. The results from Langmuir isotherm modeling agree with results from other publications.


2021 ◽  
Vol 13 (3) ◽  
pp. 1442
Author(s):  
Sanggil Park ◽  
Jaeyoung Lee ◽  
Min Bum Park

The temperature of zirconium alloy cladding on the postulated spent nuclear fuel pool complete loss of coolant accident is abruptly increased at a certain time and the cladding is almost fully oxidized to weak ZrO2 in the air. This abrupt temperature escalation phenomenon induced by the air-oxidation breakaway is called a zirconium fire. Although an air-oxidation breakaway kinetic model correlated between time and temperature has been implemented in the MELCOR code, it is likely to bring about unexpected large errors because of many limitations of model derivation. This study suggests an improved time–temperature correlated kinetic model using the Johnson–Mehl equation. It is based on that the air-oxidation breakaway is initiated by the phase transformation from the tetragonal to monoclinic ZrO2 at the oxide–metal interface in the cladding. This new model equation is also evaluated with the Zry-4 air-oxidation literature data. This equation resulted in the almost similar air-oxidation breakaway timing to the actual experimental data at 800 °C. However, at 1000 °C, it showed an error of about 8 min. This could be inferred from the influence of the ZrN phase change due to the nitrogen existing in air.


2021 ◽  
Author(s):  
Xuesong Yan ◽  
Yaling Zhang ◽  
Yucui Gao ◽  
Lei Yang

Abstract To make the nuclear fuel cycle more economical and convenient, as well as prevent nuclear proliferation, the conceptual study of a simple high-temperature dry reprocessing of spent nuclear fuel (SNF) for a ceramic fast reactor is proposed in this paper. This simple high-temperature dry (HT-dry) reprocessing includes the Atomics International Reduction Oxidation (AIROX) process and purification method for rare-earth elements. After removing the part of fission products from SNF by a HT-dry reprocessing without fine separation, the remaining nuclides and some uranium are fabricated into fresh fuel which can be used back to the ceramic fast reactor. Based on the ceramic coolant fast reactor, we studied neutron physics of nuclear fuel cycle which consists operation of ceramic reactor, removing part of fission products from SNF and preparation of fresh fuels for many time. The parameters of the study include effective multiplication factor (Keff), beam density, and nuclide mass for different ways to remove the fission products from SNF. With the increase in burnup time, the trend of increasing 239Pu gradually slows down, and the trend of 235U gradually decreases and become balanced. For multiple removal of part of fission products in the nuclear fuel cycle, the higher the removal, the larger the initial Keff.


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.


2004 ◽  
Vol 148 (3) ◽  
pp. 348-357 ◽  
Author(s):  
Yuichi Sano ◽  
Yoshihiko Shinoda ◽  
Masaki Ozawa

Author(s):  
Jerzy Narbutt

<p>Recycling of actinides from spent nuclear fuel by their selective separation followed by transmutation in fast reactors will optimize the use of natural uranium resources and minimize the long-term hazard from high-level nuclear waste. This paper describes solvent extraction processes recently developed, aimed at the separation of americium from lanthanide fission products as well as from curium present in the waste. Depicted are novel poly-N-heterocyclic ligands used as selective extractants of actinide ions from nitric acid solutions or as actinide-selective hydrophilic stripping agents.</p>


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