Browsing by Author "Le, TH"

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    Cyclic voltammetric experiment - simulation comparisons of the complex mechanism associated with electrochemical reduction of Zr4+ in LiCl-KCl eutectic molten salt
    (The Electrochemical Society, 2012-11-29) Fabian, CP; Luca, V; Le, TH; Bond, AM; Chamelot, P; Massot, L; Caravaca, C; Hanley, TL; Lumpkin, GR
    Nuclear energy increasingly represents an important option for generating largely clean CO2-free electricity and zirconium is a fission product that is expected to be present in irradiated fuels. The present investigation addresses the electrochemical reduction of Zr4+ to Zro in LiCl - KCl eutectic molten salt in the temperature range 425–550°C using cyclic voltammetry (CV), square-wave voltammetry (SWV) and bulk electrolysis. Simulations of the CV data indicate that the initial reduction proceeds through surface confined steps: Zr4+* + 2e− ↔ Zr2+* and Zr2+* + 2e− ↔ Zr* processes (* adsorbed species) followed by a peak-shaped complex diffusion controlled step that consists of a combination of closely spaced processes associated with the reactions Zr4+ + 4e− → Zro and Zr4+ + 3e− → Zr+*. Zr+*, probably in the form of ZrCl* is then further reduced to Zro* at even more negative potentials. The simulations provide the first quantitative analysis of the thermodynamics and kinetics of the Zr4+ reduction in the LiCl-KCl eutectic. © 2012, The Electrochemical Society.