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Electrostatic-thermodynamic-kinetic (ELTHEKI) modeling of the coupled \(\text {Ni}\)/\(\text {Ni}\text {O}\)/water system, under physico-chemical conditions of pressurized water reactors

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Abstract

In the present paper, we develop an electrostatic-thermodynamic-kinetic (ELTHEKI) model for studying the behavior of the specific \(\text {Ni}\)/\(\text {Ni}\text {O}\)/\(\text {H}_2\text {O}\) system, encountered in the pressurized water reactor (PWR) core. The ELTHEKI model proposes a coupled approach to describe the growth and dissolution/precipitation of the nickel oxide, under the PWR operating conditions (high temperature and alkaline pH). The electrostatic-thermodynamic-kinetic coupled modeling figures in the interfacial reaction kinetics, given by the modified Butler-Volmer (BV) law. It is expressed as a function of a composition gradient depending on the equilibrium concentration of the charge carrier, the interfacial potential drop, and the kinetic constant. Across the oxide film, nickel vacancies and holes are transported according to the Nernst-Planck (NP) equation, i.e., under concentration and potential gradients. Following the Point Defect Model (PDM), the electric field induced by charge carriers is assumed to be homogeneous within the oxide film. However, in the present study, the electric field is modeled using the Gauss law and the Helmholtz model, including also the potential drop of zero charge. Here, we propose a theoretical method for the calculation of the potential drop of zero charge at the oxide interfaces. Based on the energy band diagram, this work provides an electronic description of a metallic nickel in contact with a p-type nickel oxide, which are immersed in a liquid phase containing a redox couple. The thermodynamic aspect is also taken into account. It describes the flux between the nickel oxide and the primary fluid, driven by the deviation from an equilibrium state, which is imposed by the reactor variation conditions (pH, purification of the fluid, and temperature).

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Author notes

  1. D. You, C. Bataillon and L. Martinelli are contributed equally to this work.

Authors and Affiliations

  1. Universite Paris-Saclay, CEA, Service d’Etude du Comportement des Radionucleides, 91190, Gif-sur-Yvette, France

    T. Saidi & D. You

  2. Universite Paris-Saclay, CEA, Service de la Corrosion et du Comportement des Materiaux dans leur Environnement, 91190, Gif-sur-Yvette, France

    C. Bataillon & L. Martinelli

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Saidi, T., You, D., Bataillon, C. et al. Electrostatic-thermodynamic-kinetic (ELTHEKI) modeling of the coupled \(\text {Ni}\)/\(\text {Ni}\text {O}\)/water system, under physico-chemical conditions of pressurized water reactors. J Solid State Electrochem 27, 1119–1141 (2023). https://doi.org/10.1007/s10008-023-05385-1

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