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Radiation induced dissolution of U 3 Si 2 - A potential accident tolerant fuel
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0002-4505-0920
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.ORCID iD: 0000-0003-0663-0751
2019 (English)In: Journal of Nuclear Materials, ISSN 0022-3115, E-ISSN 1873-4820, Vol. 517, p. 263-267Article in journal (Refereed) Published
Abstract [en]

To assess the integrity of the accident tolerant fuel candidate U 3 Si 2 under geological repository conditions, the kinetics of γ-radiation- and H 2 O 2 - induced oxidative dissolution was studied. The experiments were performed in aqueous solutions containing 10 mM HCO 3 − and in solutions without added HCO 3 − . The same experiments were also performed on UO 2 for comparison. All experiments were performed using powder suspensions. The experiments show that U 3 Si 2 is less than one order of magnitude more reactive towards H 2 O 2 than is UO 2 . The dissolution yield of U 3 Si 2 slightly exceeds the theoretical yield (23%). In experiments with consecutive additions of H 2 O 2 in HCO 3 − solutions, the reactivity remains constant implying that no significant amount of a secondary phase is formed on the U 3 Si 2 surface. The dissolution of Si closely follows that of U in HCO 3 − solution. In solutions without added HCO 3 − the reactivity towards H 2 O 2 is reduced by a factor less than 2. The dissolution is slightly slower than in HCO 3 − containing solutions but precipitation of U is observed after some time. The results of consecutive additions of H 2 O 2 to the HCO 3 − free system shows that the reactivity is decreasing for every addition. This indicates that a secondary phase is formed. XRD shows that the secondary phase is studtite. The irradiation experiments show that the surface area normalized radiation chemical yields for uranium dissolution for U 3 Si 2 and UO 2 in HCO 3 − solution differ by a factor 5–10 in favour of UO 2 . This difference can largely be attributed to the difference in dissolution yield.

Place, publisher, year, edition, pages
Elsevier, 2019. Vol. 517, p. 263-267
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Chemical Sciences
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URN: urn:nbn:se:kth:diva-246447DOI: 10.1016/j.jnucmat.2019.01.023ISI: 000461048800029Scopus ID: 2-s2.0-85062038198OAI: oai:DiVA.org:kth-246447DiVA, id: diva2:1297194
Note

QC 20190319

Available from: 2019-03-19 Created: 2019-03-19 Last updated: 2019-04-03Bibliographically approved

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Maier, Annika CarolinEl Jamal, Ghada

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