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Chemical Reduction of Actinides Probed by Resonant Inelastic X-ray Scattering
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy.
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2013 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 85, no 23, 11196-11200 p.Article in journal (Refereed) Published
Abstract [en]

The study addresses the possibilities of immobilizing the mobile species of actinides in the geosphere using metallic iron. Sorption on corroding iron is well-known, but there have been uncertainties with regard to the possibilities of reducing the actinyl species to sparingly soluble oxides and, thereby, permanently immobilizing them. Resonant inelastic X-ray scattering (RIXS) measurements at the actinide 5d edges on Fe foils exposed to uranium(VI) and neptunium(V) solutions in groundwater unambigiously indicate reduction of actinides to, respectively, uranium(IV) and neptunium(IV) on iron surfaces. The reduction manifests itself in an appearance of distinct specific signatures of uranium(IV) and neptunium(IV) in the RIXS profile of 5f-5f excitations. Such signatures and RIXS intensity/cross-section behavior with varying energy of incident photons can be reproduced by model atomic-multiplet calculations of the RIXS spectra. By normalizing the RIXS signal of corresponding 5f-5f excitations to core-to-core 6p-to-5d characteristic fluorescence transitions of actinides, their reduction rates on Fe samples with different exposure to actinide solutions can be estimated. Observed reduction implies similar processes in the nuclear waste canister thus suggesting reduced probability of nuclear waste release with ground waters from the canister.

Place, publisher, year, edition, pages
2013. Vol. 85, no 23, 11196-11200 p.
National Category
Natural Sciences
URN: urn:nbn:se:uu:diva-214022DOI: 10.1021/ac4020534ISI: 000327999800007OAI: oai:DiVA.org:uu-214022DiVA: diva2:684236
Available from: 2014-01-07 Created: 2014-01-07 Last updated: 2014-01-07Bibliographically approved

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Butorin, Sergei M.Nordgren, Joseph
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Molecular and condensed matter physicsDepartment of Physics and Astronomy
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