Reactivity effects in the oxidative dissolution of UO2 nuclear fuel

Hocking, W. H.; Shoesmith, David W.; Betteridge, J.S.

doi:10.1016/0022-3115(92)90073-t

Cited by 26 publications

(11 citation statements)

References 22 publications

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“…Previous electrochemical studies of O 2 reduction on UO 2 have demonstrated how this mixed U IV /U V oxide surface is catalytic for cathodic processes [19][20][21]. The theory of Presnov and Trunov for O 2 reduction on p-type semiconductors [22][23][24], which has been used to interpret the O 2 reduction mechanism on UO 2 electrodes [19][20][21], can also be invoked to understand the mechanism of H 2 O 2 reduction. According to this theory, electron transfer to the adsorbed O 2 molecule occurs at active sites formed by adjacent cations in different valence states.…”

Section: Discussionmentioning

confidence: 99%

The electrochemical reduction of hydrogen peroxide on uranium dioxide electrodes in alkaline solution

Goldik

Noel

Shoesmith

2005

Journal of Electroanalytical Chemistry

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Section: Discussionmentioning

confidence: 99%

The electrochemical reduction of hydrogen peroxide on uranium dioxide electrodes in alkaline solution

Goldik

Noel

Shoesmith

2005

Journal of Electroanalytical Chemistry

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“…In some studies on corrosion of spent fuels under waste disposal conditions, it has been reported that UO 2 is dissolved in non-acidic solution via oxidation to UO 2þx with non-stoichiometric composition by some oxidants such as oxygen, hydrogen peroxide, and so on. [4][5][6][7][8] Actually, our recent research confirmed that dissolution of UO 2 pellet is possible even in aqueous carbonate solutions by anodic oxidation and that the resulting U(VI) species exists stably as uranyl carbonato complexes. 9,10) Under such conditions, the most of fission products (FP) should be precipitated as hydrolysates and/or insoluble carbonates.…”

Section: Introductionmentioning

confidence: 76%

Anodic Dissolution of UO2 Pellet Containing Simulated Fission Products in Ammonium Carbonate Solution

Asanuma

Harada

Nogami³

et al. 2006

J. Nucl. Sci. Technol.

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We have proposed a reprocessing process based on the dissolution of spent fuels in aqueous carbonate solution. In order to develop such a reprocessing process, anodic dissolution experiments were carried out by using a simulated spent fuel pellet in (NH 4) 2 CO 3 solution. The dissolution rate constant of the simulated fuel pellet at 323 K was estimated as 3:1Â10 À6 molÁcm À2 Ámin À1 , which is comparable to that in 5 molÁdm À3 HNO 3 solution containing 0.01 molÁ dm À3 HNO 2 at 323 K. The dissolution rate and the current efficiency for the dissolution of simulated fuel pellet in (NH 4) 2 CO 3 solution were found to decrease with the elapse of time. Furthermore, in order to examine dissolution behavior, the surface conditions of the pellet before and after the dissolution experiments were analyzed with the scanning electron microscopy and the energy dispersive X-ray spectroscopy. It was found that neat UO 2 matrix exists on the dissolved surface and a decrease in the dissolution rate and the current efficiency is caused by the increase in such surface area on the pellet. During the dissolution experiments, precipitates of the simulated fission products were observed on the pellet and in (NH 4) 2 CO 3 solution used as the electrolytic solution. Analyses of the electrolytic solution revealed that most of the simulated fission products, i.e. alkaline earth and rare earth elements, are precipitated in high ratios. From these results, it is expected that the anodic dissolution of spent fuels and the separation of fission products by precipitation can be performed simultaneously.

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“…and Nd 3? ) for U(IV) contributes to increased electrical conductivity [25]. However, recent results, presented by He et al [26], indicate that the structural changes occurring from the incorporation of fission products decrease the UO 2 dissolution rate.…”

Section: Factors Influencing the Solid Phase Reactivitymentioning

confidence: 95%

Factors influencing the rate of radiation-induced dissolution of spent nuclear fuel

2009

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Several countries plan to store spent nuclear fuel in deep geological repositories. Accurate prediction of the spent fuel dissolution rate is a key issue in the safety assessment of a future deep repository. A reliable quantitative model for radiation-induced spent fuel dissolution must be based on an accurate description of the dose distribution around the spent fuel and fundamental knowledge about the elementary processes involved. In this paper, we discuss factors influencing the rate of radiation-induced dissolution of spent nuclear fuel, focusing on solutes (H 2 , HCO 3 -, Fe(II) and organic substances affecting the H 2 O 2 concentration and factors influencing the reactivity of the fuel surface towards H 2 O 2 . Taking these factors into account, we have also simulated dissolution of spent nuclear fuel under realistic deep repository conditions.

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Reactivity effects in the oxidative dissolution of UO2 nuclear fuel

Cited by 26 publications

References 22 publications

The electrochemical reduction of hydrogen peroxide on uranium dioxide electrodes in alkaline solution

The electrochemical reduction of hydrogen peroxide on uranium dioxide electrodes in alkaline solution

Anodic Dissolution of UO2 Pellet Containing Simulated Fission Products in Ammonium Carbonate Solution

Factors influencing the rate of radiation-induced dissolution of spent nuclear fuel

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