Application of constrained Gibbs energy minimization to nuclear fuel thermochemistry

    Research output: Chapter in Book/Report/Conference proceedingConference article in proceedingsProfessional

    Abstract

    The modelling of the chemical composition of nuclear fuel is a complex problem due to the numerous fission products formed during fuel operation and their possibility to form various chemical compounds. The application of Gibbs energy minimization to model the chemical composition requires the assumption that the fuel is at local thermochemical equilibrium when the fuel is thermally in a steady state. The temperature through the pellet radius can vary 1000 K, with highest temperatures found in the pellet center. Depending on the local fuel temperature, the validity of the local equilibrium approximation varies, as diffusion and chemical kinetics limit the formation of the thermodynamically most stable species. At the fuel surface, the state of the fuel is farthest from equilibrium.

    However, with constrained Gibbs energy minimization it is possible to investigate the thermochemically most favourable state of the fuel in cases where the composition of the fuel is not at equilibrium. As a first application on nuclear fuel, the effect of cesium iodide vaporization and radiolysis in a radiation field is investigated with constrained Gibbs energy minimization. A kinetic model for cesium iodide radiolysis is used to determine a steady state, which is then used to constrain the equilibrium calculated for a nuclear fuel pellet surface. The feedback from such an analysis can be used to further refine kinetic models, as the thermochemical equilibrium calculation yields information on the possibly important species that a kinetic model should consider.
    Original languageEnglish
    Title of host publicationTopFuel 2018 Conference Proceedings (full papers)
    Number of pages10
    Publication statusPublished - 2018
    MoE publication typeD3 Professional conference proceedings
    EventTopFuel 2018: Reactor Fuel Performance - Prague, Czech Republic
    Duration: 30 Sep 20184 Oct 2018

    Conference

    ConferenceTopFuel 2018
    CountryCzech Republic
    CityPrague
    Period30/09/184/10/18

    Fingerprint

    Thermochemistry
    Nuclear fuels
    Gibbs free energy
    Cesium iodide
    Radiolysis
    Kinetics
    Nuclear fuel pellets
    Chemical analysis
    Chemical compounds
    Fission products
    Vaporization
    Reaction kinetics
    Temperature
    Feedback
    Radiation

    Cite this

    @inproceedings{688b7ed3641343ada5e1fe162cfb41e2,
    title = "Application of constrained Gibbs energy minimization to nuclear fuel thermochemistry",
    abstract = "The modelling of the chemical composition of nuclear fuel is a complex problem due to the numerous fission products formed during fuel operation and their possibility to form various chemical compounds. The application of Gibbs energy minimization to model the chemical composition requires the assumption that the fuel is at local thermochemical equilibrium when the fuel is thermally in a steady state. The temperature through the pellet radius can vary 1000 K, with highest temperatures found in the pellet center. Depending on the local fuel temperature, the validity of the local equilibrium approximation varies, as diffusion and chemical kinetics limit the formation of the thermodynamically most stable species. At the fuel surface, the state of the fuel is farthest from equilibrium.However, with constrained Gibbs energy minimization it is possible to investigate the thermochemically most favourable state of the fuel in cases where the composition of the fuel is not at equilibrium. As a first application on nuclear fuel, the effect of cesium iodide vaporization and radiolysis in a radiation field is investigated with constrained Gibbs energy minimization. A kinetic model for cesium iodide radiolysis is used to determine a steady state, which is then used to constrain the equilibrium calculated for a nuclear fuel pellet surface. The feedback from such an analysis can be used to further refine kinetic models, as the thermochemical equilibrium calculation yields information on the possibly important species that a kinetic model should consider.",
    author = "Henri Loukusa and Ville Valtavirta",
    year = "2018",
    language = "English",
    booktitle = "TopFuel 2018 Conference Proceedings (full papers)",

    }

    Loukusa, H & Valtavirta, V 2018, Application of constrained Gibbs energy minimization to nuclear fuel thermochemistry. in TopFuel 2018 Conference Proceedings (full papers)., A0127, TopFuel 2018, Prague, Czech Republic, 30/09/18.

    Application of constrained Gibbs energy minimization to nuclear fuel thermochemistry. / Loukusa, Henri; Valtavirta, Ville.

    TopFuel 2018 Conference Proceedings (full papers). 2018. A0127.

    Research output: Chapter in Book/Report/Conference proceedingConference article in proceedingsProfessional

    TY - GEN

    T1 - Application of constrained Gibbs energy minimization to nuclear fuel thermochemistry

    AU - Loukusa, Henri

    AU - Valtavirta, Ville

    PY - 2018

    Y1 - 2018

    N2 - The modelling of the chemical composition of nuclear fuel is a complex problem due to the numerous fission products formed during fuel operation and their possibility to form various chemical compounds. The application of Gibbs energy minimization to model the chemical composition requires the assumption that the fuel is at local thermochemical equilibrium when the fuel is thermally in a steady state. The temperature through the pellet radius can vary 1000 K, with highest temperatures found in the pellet center. Depending on the local fuel temperature, the validity of the local equilibrium approximation varies, as diffusion and chemical kinetics limit the formation of the thermodynamically most stable species. At the fuel surface, the state of the fuel is farthest from equilibrium.However, with constrained Gibbs energy minimization it is possible to investigate the thermochemically most favourable state of the fuel in cases where the composition of the fuel is not at equilibrium. As a first application on nuclear fuel, the effect of cesium iodide vaporization and radiolysis in a radiation field is investigated with constrained Gibbs energy minimization. A kinetic model for cesium iodide radiolysis is used to determine a steady state, which is then used to constrain the equilibrium calculated for a nuclear fuel pellet surface. The feedback from such an analysis can be used to further refine kinetic models, as the thermochemical equilibrium calculation yields information on the possibly important species that a kinetic model should consider.

    AB - The modelling of the chemical composition of nuclear fuel is a complex problem due to the numerous fission products formed during fuel operation and their possibility to form various chemical compounds. The application of Gibbs energy minimization to model the chemical composition requires the assumption that the fuel is at local thermochemical equilibrium when the fuel is thermally in a steady state. The temperature through the pellet radius can vary 1000 K, with highest temperatures found in the pellet center. Depending on the local fuel temperature, the validity of the local equilibrium approximation varies, as diffusion and chemical kinetics limit the formation of the thermodynamically most stable species. At the fuel surface, the state of the fuel is farthest from equilibrium.However, with constrained Gibbs energy minimization it is possible to investigate the thermochemically most favourable state of the fuel in cases where the composition of the fuel is not at equilibrium. As a first application on nuclear fuel, the effect of cesium iodide vaporization and radiolysis in a radiation field is investigated with constrained Gibbs energy minimization. A kinetic model for cesium iodide radiolysis is used to determine a steady state, which is then used to constrain the equilibrium calculated for a nuclear fuel pellet surface. The feedback from such an analysis can be used to further refine kinetic models, as the thermochemical equilibrium calculation yields information on the possibly important species that a kinetic model should consider.

    M3 - Conference article in proceedings

    BT - TopFuel 2018 Conference Proceedings (full papers)

    ER -