Solubility and oxidation state of uranium under anoxic conditions (N2 atmosphere)

Kaija Ollila, Markus Olin, Maija Lipponen

    Research output: Contribution to journalArticleScientificpeer-review

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    Abstract

    The UO2-matrix solubility is a critical parameter for predicting the stability of spent nuclear fuel under disposal conditions. This paper presents the results obtained from the dissolution experiments of unirradiated sintered polycrystalline UO2 pellets in deionized water, in NaHCO3 solutions, and in two different synthetic groundwaters under anoxic conditions (N2) at 25°C. The oxidation state of uranium in solution was determined experimentally using a method based on the separation of the tetravalent and hexavalent states by ion-exchange chromatography in HCl medium. The uranium contents of each fraction were analysed by ICP-MS. In order to study the controlling phase for the concentration of uranium at steady state in the solutions, a comparison of the experimental data was made with the solubilities calculated with the geochemical code EQ3/6. The measured concentrations were at the level of the solubilities of the mixed valence oxide, U4O9, in all solutions. The dominant oxidation state was the U(VI) state.
    Original languageEnglish
    Pages (from-to)9-13
    Number of pages5
    JournalRadiochimica Acta
    Volume74
    Issue numberS1
    DOIs
    Publication statusPublished - 1996
    MoE publication typeA1 Journal article-refereed

    Fingerprint

    Uranium
    uranium
    solubility
    Solubility
    atmospheres
    Oxidation
    oxidation
    spent fuels
    inductively coupled plasma mass spectrometry
    Deionized water
    nuclear fuels
    Spent fuels
    disposal
    Nuclear fuels
    chromatography
    ground water
    Chromatography
    pellets
    Oxides
    Groundwater

    Cite this

    Ollila, Kaija ; Olin, Markus ; Lipponen, Maija. / Solubility and oxidation state of uranium under anoxic conditions (N2 atmosphere). In: Radiochimica Acta. 1996 ; Vol. 74, No. S1. pp. 9-13.
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    Solubility and oxidation state of uranium under anoxic conditions (N2 atmosphere). / Ollila, Kaija; Olin, Markus; Lipponen, Maija.

    In: Radiochimica Acta, Vol. 74, No. S1, 1996, p. 9-13.

    Research output: Contribution to journalArticleScientificpeer-review

    TY - JOUR

    T1 - Solubility and oxidation state of uranium under anoxic conditions (N2 atmosphere)

    AU - Ollila, Kaija

    AU - Olin, Markus

    AU - Lipponen, Maija

    PY - 1996

    Y1 - 1996

    N2 - The UO2-matrix solubility is a critical parameter for predicting the stability of spent nuclear fuel under disposal conditions. This paper presents the results obtained from the dissolution experiments of unirradiated sintered polycrystalline UO2 pellets in deionized water, in NaHCO3 solutions, and in two different synthetic groundwaters under anoxic conditions (N2) at 25°C. The oxidation state of uranium in solution was determined experimentally using a method based on the separation of the tetravalent and hexavalent states by ion-exchange chromatography in HCl medium. The uranium contents of each fraction were analysed by ICP-MS. In order to study the controlling phase for the concentration of uranium at steady state in the solutions, a comparison of the experimental data was made with the solubilities calculated with the geochemical code EQ3/6. The measured concentrations were at the level of the solubilities of the mixed valence oxide, U4O9, in all solutions. The dominant oxidation state was the U(VI) state.

    AB - The UO2-matrix solubility is a critical parameter for predicting the stability of spent nuclear fuel under disposal conditions. This paper presents the results obtained from the dissolution experiments of unirradiated sintered polycrystalline UO2 pellets in deionized water, in NaHCO3 solutions, and in two different synthetic groundwaters under anoxic conditions (N2) at 25°C. The oxidation state of uranium in solution was determined experimentally using a method based on the separation of the tetravalent and hexavalent states by ion-exchange chromatography in HCl medium. The uranium contents of each fraction were analysed by ICP-MS. In order to study the controlling phase for the concentration of uranium at steady state in the solutions, a comparison of the experimental data was made with the solubilities calculated with the geochemical code EQ3/6. The measured concentrations were at the level of the solubilities of the mixed valence oxide, U4O9, in all solutions. The dominant oxidation state was the U(VI) state.

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    JO - Radiochimica Acta

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    SN - 0033-8230

    IS - S1

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