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The relative stabilities of the compounds in the binary Pd-Si system were assessed using firstprinciples calculations and experimental methods. Calculations of lattice parameters and enthalpy of formation indicate that Pd5Si, Pd9Si2, Pd3Si, Pd2Si, and PdSi are the stable phases at 0 K. X-ray diffraction analyses (XRD) and electron probe microanalysis (EPMA) of as-solidified and heat-treated samples support the computational findings, except that the PdSi phase was not observed at low temperature. Considering both experimental data and first-principles results, the compounds Pd5Si, Pd9Si2, Pd3Si, and Pd2Si are treated as stable phases all way to zero kelvin while the PdSi is stable over a limited range, exhibiting a lower bound. Using these findings, a comprehensive solution-based thermodynamic model is formulated for the Pd-Si system, permitting phase diagram calculation. The liquid phase is described using a three-species association model and other phases are treated as solid solutions, where a random substitutional model is adopted for Pd-fcc and Si-dia, and a two-sublattice model is employed for Pd5Si, Pd9Si2, Pd3Si, Pd2Si , and PdSi. Model parameters are fitted using available experimental data and first-principles data, and the resulting phase diagram is reported over the full range of compositions.

Phase selection and microstructure in directional solidification of glass forming Pd-Si-Cu alloys