Thermodynamic evaluation of liquid-gas surface tension for $U-O-ZR$ mixtures using the butler equation
Abstract
In this work, the Butler equation is assessed for evaluating the liquid/gas surface tension for three
compositions in the ternary $U −Zr−O$ system over a wide temperature range 2600−3100 K. In this
approach, the liquid phase Gibbs energy is obtained from two CALPHAD-type databases, NUCLEA
and TAF-ID. Two formulations of the Butler equation makes use of an ideal phase mixing hypothesis
(φ being the weighting factor) with and without surface tension laws for pure components. A third
formulation corresponds to the classical form of the Butler equation found in the literature where the
interfacial Gibbs excess energy is assumed to be proportional to to the liquid one (the multiplicative
factor $k_Γ$ being related to the ratio of broken bounds). Computed surface tensions are compared
to experimental values obtained by C. Denier in her Ph.D. thesis in the VITI facility at CEA
Cadarache. Three different compositions corresponding to different Zirconium oxydation degree,
C0, C30 and C50 are considered. It is shown through a limited parametric analysis that the choice
of the CALPHAD database affects both the slope w.r.t temperature and the level of the interfacial
energy while parameters $\phi$ and $k_Γ$ mainly affects the level and only slightly the slope. Considering
pure component surface tension data has a significant impact on both and, considering the C0
composition measurements, it is shown that parameters $\phi$ and $k_Γ$ can be successfully calibrated for
reproducing these data. However, the steep variation of the interfacial energy w.r.t temperature
exhibited by experimental results for the C30 composition is, in any case, not correctly captured.
This shows the need for further improvement of the liquid thermodynamic modelling and a path
forward is proposed.
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Physics [physics]Origin | Files produced by the author(s) |
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