Oxidative Corrosion of the UO2 (001) Surface by Nonclassical Diffusion
Uranium oxide is central to every stage of the nuclear fuel cycle, from mining through fuel fabrication and use, to waste disposal and environmental cleanup. Its chemical and mechanical stability are intricately linked to the concentration of interstitial O atoms within the structure and the oxidati...
Publié dans: | Langmuir : the ACS journal of surfaces and colloids. - 1985. - 33(2017), 46 vom: 21. Nov., Seite 13189-13196 |
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Auteur principal: | |
Autres auteurs: | , , , , , |
Format: | Article en ligne |
Langue: | English |
Publié: |
2017
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Accès à la collection: | Langmuir : the ACS journal of surfaces and colloids |
Sujets: | Journal Article Research Support, U.S. Gov't, Non-P.H.S. |
Résumé: | Uranium oxide is central to every stage of the nuclear fuel cycle, from mining through fuel fabrication and use, to waste disposal and environmental cleanup. Its chemical and mechanical stability are intricately linked to the concentration of interstitial O atoms within the structure and the oxidation state of U. We have previously shown that, during corrosion of the UO2 (111) surface under either 1 atm of O2 gas or oxygenated water at room temperature, oxygen interstitials diffuse into the substrate to form a superlattice with three-layer periodicity. In the current study, we present results from surface X-ray scattering that reveal the structure of the oxygen diffusion profile beneath the (001) surface. The first few layers below the surface oscillate strongly in their surface-normal lattice parameters, suggesting preferential interstitial occupation of every other layer below the surface, which is geometrically consistent with the interstitial network that forms below the oxidized (111) surface. Deeper layers are heavily contracted and indicate that the oxidation front penetrates ∼52 Å below the (001) surface after 21 days of dry O2 gas exposure at ambient pressure and temperature. X-ray photoelectron spectroscopy indicates U is present as U(IV), U(V), and U(VI) |
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Description: | Date Completed 31.07.2018 Date Revised 31.07.2018 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1520-5827 |
DOI: | 10.1021/acs.langmuir.7b02800 |