UO dissolution in bicarbonate solution with HO; The Effect of temperature

McGrady, J.; Kumagai, Yuta; Kitatsuji, Yoshihiro; Kirishima, Akira*; Akiyama, Daisuke*; Watanabe, Masayuki

RSC Advances (Internet), 13(40), p.28021 - 28029, 2023/09

https://doi.org/10.1039/D2RA08131H

Upon nuclear waste canister failure and contact of spent nuclear fuel with groundwater, the UO matrix of spent fuel will interact with oxidants in the groundwater generated by water radiolysis. Bicarbonate (HCO) is often found in groundwater, and the HO induced oxidative dissolution of UO in bicarbonate solution has previously been studied under various conditions. Temperatures in the repository at the time of canister failure will differ depending on the location, yet the effect of temperature on oxidative dissolution is unknown. To investigate, the decomposition rate of HO at the UO surface and dissolution of U in bicarbonate solution (0.1, 1, 10 and 50 mM) was analysed at various temperatures (10, 25, 45 and 60 C). At [HCO] 1 mM, the apparent equilibrium concentration of U decreased with increasing temperature. This was attributed to the formation of U-bicarbonate species at the surface and a change in the mechanism of HO decomposition from oxidative to catalytic. At 0.1 mM, no obvious correlation between temperature and U dissolution was observed, and thermodynamic calculations indicated this was due to a change in the surface species. A pathway to explain the observed dissolution behaviour of UO in bicarbonate solution as a function of temperature was proposed.

Thorium oxide dissolution in HNO-HF mixture; Kinetics and mechanism

Simonnet, M.; Barr, N.*; Drot, R.*; Le Naour, C.*; Sladkov, V.*; Delpech, S.*

Radiochimica Acta, 107(4), p.289 - 297, 2019/04

https://doi.org/10.1515/ract-2018-3052

Effects of OH activity and temperature on the dissolution rate of compacted montmorillonite under highly alkaline conditions

Sawaguchi, Takuma; Tsukada, Manabu; Yamaguchi, Tetsuji; Mukai, Masayuki

Clay Minerals, 51(2), p.267 - 278, 2016/05

https://doi.org/10.1180/claymin.2016.051.2.12

The dependences of the dissolution rate of compacted montmorillonite on activity of OH (a-) and temperature (T) were investigated. The dissolution rate of montmorillonite () in compacted pure montmorillonite, which was formulized as = 10 (a-) e, was higher than that in the compacted sand-bentonite mixtures: = 3500 (a-) e. The difference can be explained by considering the decrease in a- in the mixtures accompanied by dissolution of accessory minerals such as quartz and chalcedony. The dissolution rate model developed for pure montmorillonite is expected to be applied to bentonite mixtures if quantification of the decrease in a- is achieved somehow.

An Investigation into dissolution rate of spent nuclear fuel in aqueous reprocessing

Mineo, Hideaki; Isogai, Hikaru; Morita, Yasuji; Uchiyama, Gunzo*

Journal of Nuclear Science and Technology, 41(2), p.126 - 134, 2004/02

https://doi.org/10.3327/jnst.41.126

A simple equation was proposed for the dissolution rate of spent LWR fuel, of which the change in the dissolution area was estimated by taking into account of the area of the cracks occurring due to thermal shrinkage of the pellets during irradiation. The applicability of proposed equation was examined using LWR fuel dissolution test results in the present study as well as the results obtained by other workers. The equation showed good agreements with the dissolution test results obtained from spent fuel pellets and pulverized spent fuel. It was indicated that the proposed equation was simple and would be useful for the prediction of dissolution of spent LWR fuels. However, the initial effective dissolution area, the parameter of the equation, was found to depend on the temperature, which could not be explained by the proposed equation. Further studies on the role of other factors affecting dissolution rate, such as nitrous acid, in the dissolution of spent fuel was required.

Characteristics of MOX dissolution with silver mediated electrolytic oxidation method

Umeda, Miki; Nakazaki, Masato; Kida, Takashi; Sato, Kenji; Kato, Tadahito; Kihara, Takehiro; Sugikawa, Susumu

JAERI-Tech 2003-024, 23 Pages, 2003/03

JAERI-Tech-2003-024.pdf:0.98MB

MOX dissolution with silver mediated electrolytic oxidation method is planned for the preparation of plutonium nitrate solution to be used for criticality safety experiments at Nuclear Fuel Cycle Safety Engineering Research Facility (NUCEF). Silver mediated electrolytic oxidation method uses the strong oxidisation ability of Ag(II) ion. This method is thought to be effective for the dissolution of MOX, which is difficult to be dissolved with nitric acid.In this paper, the results of experiments on dissolution with 100 g of MOX are described. It was confirmed by the results that the MOX powder to be used at NUCEF was completely dissolved by silver mediated electrolytic oxidation method and that Pu(VI) ion in the obtained solution was reduced to tetravalent by means of NO purging.