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Impact of Stoichiometry on the Mechanism and Kinetics of Oxidative Dissolution of UO 2 Induced by H 2 O 2 and γ-Irradiation
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0552-6282
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0663-0751
2019 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 123, no 15, p. 9919-9925Article in journal (Refereed) Published
Abstract [en]

Radiation-induced oxidative dissolution of uranium dioxide (UO 2 ) is one of the most important chemical processes of U driven by redox reactions. We have examined the effect of UO 2 stoichiometry on the oxidative dissolution of UO 2 in aqueous sodium bicarbonate solution induced by hydrogen peroxide (H 2 O 2 ) and γ-ray irradiation. By comparing the reaction kinetics of H 2 O 2 between stoichiometric UO 2.0 and hyper-stoichiometric UO 2.3 , we observed a significant difference in reaction speed and U dissolution kinetics. The stoichiometric UO 2.0 reacted with H 2 O 2 much faster than the hyper-stoichiometric UO 2.3 . The U dissolution from UO 2.0 was initially much lower than that from UO 2.3 but gradually increased as the oxidation by H 2 O 2 proceeded. Increase in the initial H 2 O 2 concentration caused decrease in the U dissolution yield with respect to the H 2 O 2 consumption both for UO 2.0 and UO 2.3 . This decrease in the U dissolution yield is attributed to the catalytic decomposition of H 2 O 2 on the surface of UO 2 . The γ-ray irradiation induced the U dissolution that is analogous to the kinetics by the exposure to a low concentration (2 × 10 -4 mol dm -3 ) of H 2 O 2 . The exposure to higher H 2 O 2 concentrations caused lower U dissolution and resulted in deviation from the U dissolution behavior by γ-ray irradiation.

Place, publisher, year, edition, pages
American Chemical Society , 2019. Vol. 123, no 15, p. 9919-9925
Keywords [en]
Dissolution, Irradiation, Kinetics, Reaction kinetics, Redox reactions, Sodium bicarbonate, Stoichiometry, Uranium dioxide, Bicarbonate solution, Catalytic decomposition, Dissolution behavior, Dissolution kinetics, Gamma-ray irradiation, Low concentrations, Mechanism and kinetics, Oxidative dissolution, Gamma rays
National Category
Other Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-255911DOI: 10.1021/acs.jpcc.9b00862Scopus ID: 2-s2.0-85064646707OAI: oai:DiVA.org:kth-255911DiVA, id: diva2:1344854
Note

QC 20190822

Available from: 2019-08-22 Created: 2019-08-22 Last updated: 2019-08-22Bibliographically approved

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Barreiro Fidalgo, AlexandreJonsson, Mats

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