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The role of surface-bound hydroxyl radicals in the reaction between H2O2 and UO2
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).ORCID iD: 0000-0003-0552-6282
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH).ORCID iD: 0000-0003-0663-0751
2018 (English)In: Journal of coordination chemistry (Print), ISSN 0095-8972, E-ISSN 1029-0389, Vol. 71, no 11-13, p. 1799-1807Article in journal (Refereed) Published
Abstract [en]

In this work, we have studied the reaction between H2O2 and UO2 with particular focus on the nature of the hydroxyl radical formed as an intermediate. Experiments were performed to study the kinetics of H2O2 consumption and uranium dissolution at different initial H2O2 concentrations. The results show that the consumption rates at a given H2O2 concentration are different depending on the initial H2O2 concentration. This is attributed to an alteration of the reactive interface, likely caused by blocking of surface sites by oxidized U/surface-bound hydroxyl radicals. The dissolution yield given by the amount of dissolved uranium divided by the amount of consumed hydrogen peroxide was used to compare the different cases. For all initial H2O2 concentrations, the dissolution yield increases with reaction time. The final dissolution yield decreases with increasing initial H2O2 concentration. This is expected from the mechanism of catalytic decomposition of H2O2 on oxide surfaces. As the experiments were performed in solutions containing 10mM H2O2 and a strong concentration dependence was observed in the 0.2-2.0mM H2O2 concentration range, we conclude that the intermediate hydroxyl radical is surface bound rather than free.

Place, publisher, year, edition, pages
2018. Vol. 71, no 11-13, p. 1799-1807
Keywords [en]
Hydroxyl radical; H2O2; UO2; catalysis; surface
National Category
Chemical Sciences Inorganic Chemistry
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-261430DOI: 10.1080/00958972.2018.1466287ISI: 000448334400014OAI: oai:DiVA.org:kth-261430DiVA, id: diva2:1358496
Note

QC20191008

Available from: 2019-10-07 Created: 2019-10-07 Last updated: 2019-10-08Bibliographically approved

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Barreiro Fidalgo, AlexandreJonsson, Mats
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