Dissolution of spent nuclear fuel in carbonate–peroxide solution

Soderquist, Chuck Z.; Hanson, Brady D.

doi:10.1016/j.jnucmat.2009.11.001

Cited by 35 publications

(23 citation statements)

References 13 publications

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“…The fuel was extracted from its Zircaloy cladding by mechanical means. Because of the strong bond between the rim of the irradiated fuel and the zirconium sheath and Zircaloy cladding, it was likely that the extracted sample did not contain a significant amount of the cladding metals [24,25]. Once removed from the cladding the material was crushed prior to any processing.…”

Section: Samplingmentioning

confidence: 99%

Nanostructure of metallic particles in light water reactor used nuclear fuel

Buck

Mausolf

McNamara

et al. 2015

Journal of Nuclear Materials

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An extraordinary nano-structure has been observed in the metallic (Mo-Tc-Ru-Rh-Pd) particles that are known to form during irradiated in light water nuclear reactor fuels. This structure points possible high catalytic reactivity through the occurrence of a very high surface area as well as defect sites. We have analyzed separated metallic particles from dissolved high burn-up spent nuclear fuel using scanning and transmission electron microscopy. The larger particles vary in diameter between ~10 and ~300 nm and possess a hexagonally close packed epsilon-ruthenium structure. These particles are not always single crystals but often consist of much smaller crystallites on the order of 1-3 nm in diameter with evidence suggesting the occurrence of some amorphous regions. It is possible that neutron irradiation and fission product recoils generated the unusual small crystallite size. The composition of the metallic particles was variable with low levels of uranium present in some of the particles. We hypothesize that the uranium may have induced the formation of the amorphous (or frustrated) metal structure. This unique nanostructure may play an important role in the environmental behavior of nuclear fuels.

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Section: Samplingmentioning

confidence: 99%

Nanostructure of metallic particles in light water reactor used nuclear fuel

Buck

Mausolf

McNamara

et al. 2015

Journal of Nuclear Materials

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“…However, the working voltage is different due to the lower redox potential of sodium compared with lithium. 27 Li + , however, is considered to be involved in the electrochemical ion-transfer reactions. 294 and 212 mA h g À1 , respectively, with the coulombic efficiency of 72.1%, whereas, both charge and discharge capacity fades with increasing cycle numbers and the capacity retention equals to 55.2% aer 50 cycles.…”

Section: Resultsmentioning

confidence: 99%

High capacity and rate capability of a layered Li₂RuO₃cathode utilized in hybrid Na⁺/Li⁺batteries

et al. 2015

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A novel hybrid Na + /Li + battery is established by using Li 2 RuO 3 as the cathode, 1 M NaClO 4 in 1 : 1 EC/PC solution as the electrolyte and metallic sodium as the anode. In the working voltages between 2.0 and 4.0 V, Li 2 RuO 3 delivers a high discharge capacity of 168 mA h g À1 under the current density of 0.1 A g À1 and an excellent capacity retention of about 88.1% after 50 cycles. The cathode also exhibits superior rate capability and long-term cycle life, whose discharge capacity reaches 85 mA h g À1 after 300 cycles at the current density of 1 A g À1 . Importantly, both Na + and Li + can reversibly intercalate/deintercalate into Li 2 RuO 3 in the same manner as in the typical Li-ion half cell. In addition, ex situ X-ray diffraction patterns of the initial charge and discharge processes as well as after long electrochemical cycles are examined to study its structural evolution. Our studies provide a strong insight into the design and application of novel rechargeable batteries.

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“…The composition of the insoluble residues depends mainly on the dissolution conditions, especially nitric acid concentration, but also on the time elapsed between the end of dissolution and the clarification of the dissolver solution 16 . The amount of insoluble residues increases with the fission yield and therefore depends on the initial fuel composition and the burn-up 14,20 .…”

Section: Introductionmentioning

confidence: 99%

Microstructural evolution of UO2 pellets containing metallic particles of Ru, Rh and Pd during dissolution in nitric acid solution: 3D-ESEM monitoring

et al. 2019

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Uranium dioxide containing 3 mol.% platinum group metals (PGMs) (Ru, Rh, Pd) was synthesized by hydroxide precipitation. The powders were converted to oxides, pelletized and sintered to prepare dense pellets of UO 2 incorporating PGMs particles. The characterization techniques performed revealed a microstructure similar to that of spent nuclear fuel (SNF). Dissolution tests in nitric acid demonstrated that in the presence of PGMs, the uranium dissolution rate was increased and the induction period was shortened. We used a new method based on the acquisition of Environmental Scanning Electron Microscopy (ESEM) micrographs recorded at three tilt angles and at different dissolution times. This method allowed the reconstruction of the topography of the solid/liquid interface. By monitoring the evolution of the solid/liquid interface during dissolution by means of 3D reconstructions, we were able to observe preferential dissolution zones in the vicinity of the PGMs particles and to determine microscopic dissolution rates for several regions of interest. PGMs particles were found mainly at the grain boundaries. In 0.1 M HNO 3 solution at 60˚C, the normalized dissolution rate for uranium at the grain boundaries reached R L (U) = (7 ± 1)×10-2 g.m-2 .d-1 , a value similar to the normalized dissolution rate determined for the whole image over the first 30 days of the experiment. This result showed that the dissolution occurred mainly at the UO 2 grain boundaries in the vicinity of PGMs particles. Furthermore, the 3D reconstructions of the solid/liquid interface were used to determine the evolution of the surface area of the pellet. By combining the weight losses determined at the macroscopic scale using the uranium concentrations in solution with the reactive surface area values, it was possible to estimate an effective normalized dissolution rate for the whole pellet.

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Dissolution of spent nuclear fuel in carbonate–peroxide solution

Cited by 35 publications

References 13 publications

Nanostructure of metallic particles in light water reactor used nuclear fuel

Nanostructure of metallic particles in light water reactor used nuclear fuel

High capacity and rate capability of a layered Li₂RuO₃cathode utilized in hybrid Na⁺/Li⁺batteries

Microstructural evolution of UO2 pellets containing metallic particles of Ru, Rh and Pd during dissolution in nitric acid solution: 3D-ESEM monitoring

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Dissolution of spent nuclear fuel in carbonate–peroxide solution

Cited by 35 publications

References 13 publications

Nanostructure of metallic particles in light water reactor used nuclear fuel

Nanostructure of metallic particles in light water reactor used nuclear fuel

High capacity and rate capability of a layered Li2RuO3cathode utilized in hybrid Na+/Li+batteries

Microstructural evolution of UO2 pellets containing metallic particles of Ru, Rh and Pd during dissolution in nitric acid solution: 3D-ESEM monitoring

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Product

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High capacity and rate capability of a layered Li₂RuO₃cathode utilized in hybrid Na⁺/Li⁺batteries