Oxidation of UO2 by radiolytic oxidants

Ekeroth, Ella; Jönsson, Mats

doi:10.1016/j.jnucmat.2003.07.001

Cited by 98 publications

(108 citation statements)

References 15 publications

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“…To the best of our knowledge, second order rate constants for oxidation of UO 2 have only been reported in a very limited number of publications so far [39,40]. In reference [39] 6 2-.…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

“…In reference [39] 6 2-. Interestingly, the logarithm of the rate constant for these oxidants was found to be linearly related to the one-electron reduction potential of the oxidant.…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

“…Electrochemical studies indicate that H 2 O 2 is approximately 200 times more reactive than O 2 [42]. The relative reactivity estimated from the relationship between rate constant and one-electron reduction potential also gives a factor of 200 when comparing these two oxidants [39].…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

“…Hence, the oxidation of UO 2 by these oxidants will be a stepwise process in which the first single electron transfer is rate limiting. The mechanism for UO 2 oxidation by H 2 O 2 as suggested in reference [39] is described by reactions (5) and (6).…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

“…The concentration of H 2 will be many orders of magnitude higher but the reactivity is low and the reduction by H 2 often requires a catalyst. Numerous studies, aiming at elucidating the mechanistic details as well as the kinetics of radiation induced dissolution of UO 2 , have been performed [30][31][32][33][34][35][36][37][38][39][40][41][42]. Owing to the intrinsic complexity of the system, it has been difficult to draw general conclusions from studies on real spent nuclear fuel.…”

Section: Introductionmentioning

confidence: 99%

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Oxidation of UO2(s) in aqueous solution

Roth

Jönsson

2008

Open Chemistry

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Abstract:In this review the kinetics and mechanism of oxidative dissolution of UO 2 (s), mainly under conditions of relevance for the safety assessment of a deep geological repository for spent nuclear fuel, are discussed. Rate constants for the elementary processes involved (oxidation of UO 2 and dissolution of oxidized UO 2 ) are used to calculate the rates of oxidative UO 2 (s) dissolution under various conditions (type of oxidant, oxidant concentration and HCO 3 -/CO 3 2-concentration) for which experimental data are also available. The calculated rates are compared to the corresponding experimental values under the assumption that the experimental numbers reflect the steady-state conditions of the system. The agreement between the calculated rates and the corresponding experimental ones is very good, in particular for the higher rates. In general, the calculated rates are somewhat higher than the experimental numbers. This can be due partly to the use of initial concentrations rather than steady-state concentrations in the calculations. The kinetic data are also used to quantitatively discuss the dynamics of spent nuclear fuel dissolution under deep geological repository conditions. © Versita Warsaw and Springer-Verlag Berlin Heidelberg.

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“…To the best of our knowledge, second order rate constants for oxidation of UO 2 have only been reported in a very limited number of publications so far [39,40]. In reference [39] 6 2-.…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

“…In reference [39] 6 2-. Interestingly, the logarithm of the rate constant for these oxidants was found to be linearly related to the one-electron reduction potential of the oxidant.…”

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

Section: Oxidation Of Uo 2 (S)mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Oxidation of UO2(s) in aqueous solution

Roth

Jönsson

2008

Open Chemistry

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An Overview of Interfacial Radiation Chemistry in Nuclear Technology

Jönsson

2014

Israel Journal of Chemistry

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Interfacial radiation chemistry is of key importance in nuclear technology because most materials in the vicinity of radioactive materials in nuclear power plants, reprocessing plants, and repositories for nuclear waste are exposed to ionizing radiation. Corrosion is a crucial issue for the long‐term performance and safety of these installations. Nevertheless, this field is still fairly undeveloped. In this paper, the current state of the art with particular focus on reactions between aqueous radiolysis products and metal or metal oxide surfaces is discussed. The general reactivity of hydrogen peroxide and the hydroxyl radical towards oxide surfaces is discussed on the basis of recent experimental results and DFT calculations. More specific discussions on radiation‐induced surface processes in a future geological repository for spent nuclear fuel are given as relevant examples. This includes radiation‐induced dissolution of spent nuclear fuel in contact with groundwater, radiation‐induced corrosion of copper, and radiation‐induced alterations of bentonite clay. Current knowledge gaps in these areas are highlighted.

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In situ Raman monitoring of materials under irradiation: study of uranium dioxide alteration by water radiolysis

Canizarès

Guimbretière

Tobon

et al. 2012

J Raman Spectroscopy

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In situ Raman scattering studies allow following real-time evolutions of volume or surface structures under extreme conditions. In nuclear materials sciences, ion irradiation-induced atomic organization modification and water radiolysis are of a major interest. In order to better understand these phenomena, we have developed an in situ versatile portable Raman spectroscopy system coupled with a cyclotron accelerator, allowing monitoring of a solid/liquid interface under irradiation and thus giving access to effects of radiolysis. The different parts of the system and their improvements are described in details.The system efficiency is highlighted by a comparative study of the time dependence of UO 2 surface modification induced, on one hand by contact with water under irradiation by 5 MeV He 2+ particles, and on the other hand by pure chemical alteration, through contact with a hydrogen peroxide solution.

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Oxidation of UO2 by radiolytic oxidants

Cited by 98 publications

References 15 publications

Oxidation of UO2(s) in aqueous solution

Oxidation of UO2(s) in aqueous solution

An Overview of Interfacial Radiation Chemistry in Nuclear Technology

In situ Raman monitoring of materials under irradiation: study of uranium dioxide alteration by water radiolysis

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