A Calphad-compatible method to calculate liquid/liquid interfacial energies in immiscible metallic systems

Abstract

For the calculation of liquid/liquid interfacial energies in monotectic metallic alloys only simplified models are known, which suppose the validity of the regular solution model for the liquid solution. In the present paper a Calphad-compatible method is developed to calculate the liquid/liquid interfacial energies in binary, ternary and multicomponent liquid monotectic alloys. The method can be considered as the extension of the Butler equation to the liquid/liquid interfaces. The first order interfacial phase transition has been predicted at a certain critical temperature, which is about 18% of the bulk critical temperature. Below this critical temperature the compositions of the two sides of the liquid/liquid interface are different, while above this critical temperature the compositions at the two sides of the interface are identical. The latter case is valid for the majority of liquid metallic systems above their monotectic temperatures. The method has been validated against the experimentally measured liquid/liquid interfacial energies in the Ga–Pb and Al–Bi systems. The method is found to be very sensitive to the correctness of the Calphad-assessment of the partial excess Gibbs energies of the components in the liquid solution. The excess Gibbs energy function of the liquid Al–Bi solution was reassessed using our recent exponential temperature dependence of the interaction energies.