Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation

Petri Kinnunen, Martin Bojinov, Jarmo Lehikoinen, Klas Lundgren

    Research output: Chapter in Book/Report/Conference proceedingChapter or book articleProfessional

    Abstract

    The ultimate goal of this work is to develop a deterministic model for activity build-up and to increase the theoretical understanding of the oxide film build-up and breakdown, controlling the localised corrosion of structural materials in Light Water Reactors. The first step of the overall reaction of activity build-up in oxidised structural material surfaces in primary LWR circuits is the interaction of activated ionic species from the coolant with the oxide layers, involving surface complexation and redeposition stages. An experimental investigation of the interaction of the LWR oxides with coolant-originating species was performed to assess the thermodynamics of these stages. A series of high-temperature titrations at 280oC was performed, in which the competitive adsorptivity of Zn, Co and Ni cations onto iron oxide surfaces has been studied. The experiments provided the necessary information concerning the reactions at outer oxide / coolant interface. The obtained results were quantitatively interpreted using the diffuse layer and non-electrical surface complexation models and the extracted stability constants of the surface complexes were found to be in agreement with extrapolations of room-temperature data. The determination of the kinetic and transport parameters for the subsequent incorporation of Zn in the inner oxide layer on stainless steels and nickel alloys is based on the fitting of experimental depth profiles of these elements to the diffusion-migration equations for the non-steady state transport. The obtained parameter values are discussed in terms of the dynamics of the oxides on the structural materials.
    Original languageEnglish
    Title of host publicationSAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006
    Subtitle of host publicationFinal Report
    Place of PublicationEspoo
    PublisherVTT Technical Research Centre of Finland
    Pages115-126
    ISBN (Electronic)951-38-6887-7
    ISBN (Print)951-38-6886-9
    Publication statusPublished - 2006
    MoE publication typeNot Eligible

    Publication series

    SeriesVTT Tiedotteita - Research Notes
    Number2363
    ISSN1235-0605

    Fingerprint

    oxide films
    coolants
    conduction
    oxides
    adsorptivity
    light water reactors
    nickel alloys
    iron oxides
    titration
    extrapolation
    stainless steels
    surface layers
    corrosion
    breakdown
    interactions
    cations
    thermodynamics
    kinetics
    room temperature
    profiles

    Cite this

    Kinnunen, P., Bojinov, M., Lehikoinen, J., & Lundgren, K. (2006). Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation. In SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006: Final Report (pp. 115-126). Espoo: VTT Technical Research Centre of Finland. VTT Tiedotteita - Research Notes, No. 2363
    Kinnunen, Petri ; Bojinov, Martin ; Lehikoinen, Jarmo ; Lundgren, Klas. / Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation. SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006: Final Report. Espoo : VTT Technical Research Centre of Finland, 2006. pp. 115-126 (VTT Tiedotteita - Research Notes; No. 2363).
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    abstract = "The ultimate goal of this work is to develop a deterministic model for activity build-up and to increase the theoretical understanding of the oxide film build-up and breakdown, controlling the localised corrosion of structural materials in Light Water Reactors. The first step of the overall reaction of activity build-up in oxidised structural material surfaces in primary LWR circuits is the interaction of activated ionic species from the coolant with the oxide layers, involving surface complexation and redeposition stages. An experimental investigation of the interaction of the LWR oxides with coolant-originating species was performed to assess the thermodynamics of these stages. A series of high-temperature titrations at 280oC was performed, in which the competitive adsorptivity of Zn, Co and Ni cations onto iron oxide surfaces has been studied. The experiments provided the necessary information concerning the reactions at outer oxide / coolant interface. The obtained results were quantitatively interpreted using the diffuse layer and non-electrical surface complexation models and the extracted stability constants of the surface complexes were found to be in agreement with extrapolations of room-temperature data. The determination of the kinetic and transport parameters for the subsequent incorporation of Zn in the inner oxide layer on stainless steels and nickel alloys is based on the fitting of experimental depth profiles of these elements to the diffusion-migration equations for the non-steady state transport. The obtained parameter values are discussed in terms of the dynamics of the oxides on the structural materials.",
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    year = "2006",
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    Kinnunen, P, Bojinov, M, Lehikoinen, J & Lundgren, K 2006, Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation. in SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006: Final Report. VTT Technical Research Centre of Finland, Espoo, VTT Tiedotteita - Research Notes, no. 2363, pp. 115-126.

    Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation. / Kinnunen, Petri; Bojinov, Martin; Lehikoinen, Jarmo; Lundgren, Klas.

    SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006: Final Report. Espoo : VTT Technical Research Centre of Finland, 2006. p. 115-126 (VTT Tiedotteita - Research Notes; No. 2363).

    Research output: Chapter in Book/Report/Conference proceedingChapter or book articleProfessional

    TY - CHAP

    T1 - Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation

    AU - Kinnunen, Petri

    AU - Bojinov, Martin

    AU - Lehikoinen, Jarmo

    AU - Lundgren, Klas

    PY - 2006

    Y1 - 2006

    N2 - The ultimate goal of this work is to develop a deterministic model for activity build-up and to increase the theoretical understanding of the oxide film build-up and breakdown, controlling the localised corrosion of structural materials in Light Water Reactors. The first step of the overall reaction of activity build-up in oxidised structural material surfaces in primary LWR circuits is the interaction of activated ionic species from the coolant with the oxide layers, involving surface complexation and redeposition stages. An experimental investigation of the interaction of the LWR oxides with coolant-originating species was performed to assess the thermodynamics of these stages. A series of high-temperature titrations at 280oC was performed, in which the competitive adsorptivity of Zn, Co and Ni cations onto iron oxide surfaces has been studied. The experiments provided the necessary information concerning the reactions at outer oxide / coolant interface. The obtained results were quantitatively interpreted using the diffuse layer and non-electrical surface complexation models and the extracted stability constants of the surface complexes were found to be in agreement with extrapolations of room-temperature data. The determination of the kinetic and transport parameters for the subsequent incorporation of Zn in the inner oxide layer on stainless steels and nickel alloys is based on the fitting of experimental depth profiles of these elements to the diffusion-migration equations for the non-steady state transport. The obtained parameter values are discussed in terms of the dynamics of the oxides on the structural materials.

    AB - The ultimate goal of this work is to develop a deterministic model for activity build-up and to increase the theoretical understanding of the oxide film build-up and breakdown, controlling the localised corrosion of structural materials in Light Water Reactors. The first step of the overall reaction of activity build-up in oxidised structural material surfaces in primary LWR circuits is the interaction of activated ionic species from the coolant with the oxide layers, involving surface complexation and redeposition stages. An experimental investigation of the interaction of the LWR oxides with coolant-originating species was performed to assess the thermodynamics of these stages. A series of high-temperature titrations at 280oC was performed, in which the competitive adsorptivity of Zn, Co and Ni cations onto iron oxide surfaces has been studied. The experiments provided the necessary information concerning the reactions at outer oxide / coolant interface. The obtained results were quantitatively interpreted using the diffuse layer and non-electrical surface complexation models and the extracted stability constants of the surface complexes were found to be in agreement with extrapolations of room-temperature data. The determination of the kinetic and transport parameters for the subsequent incorporation of Zn in the inner oxide layer on stainless steels and nickel alloys is based on the fitting of experimental depth profiles of these elements to the diffusion-migration equations for the non-steady state transport. The obtained parameter values are discussed in terms of the dynamics of the oxides on the structural materials.

    M3 - Chapter or book article

    SN - 951-38-6886-9

    T3 - VTT Tiedotteita - Research Notes

    SP - 115

    EP - 126

    BT - SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006

    PB - VTT Technical Research Centre of Finland

    CY - Espoo

    ER -

    Kinnunen P, Bojinov M, Lehikoinen J, Lundgren K. Further development of the Mixed-Conduction Model of oxide films in LWRs emphasising surface complexationand reprecipitation. In SAFIR: The Finnish Research Programme on Nuclear Power Plant Safety 2003-2006: Final Report. Espoo: VTT Technical Research Centre of Finland. 2006. p. 115-126. (VTT Tiedotteita - Research Notes; No. 2363).