A prediction of the thermodynamic, thermophysical, and mechanical properties of CrTaO₄ from first principles

It is reported that the self-forming CrTaO₄ oxide scale can protect refractory high-entropy alloys from oxidation, superior to Cr₂O₃. In this paper, the phase stability, mechanical, and thermal properties of three polymorphous phases of CrTaO₄ are systematically investigated from first-principles density functional theory calculations. The mechanical properties predicted using the strain–energy methods indicated that all three phases are mechanically stable. The temperature dependence of elastic constants and polycrystalline moduli of three phases demonstrated the thermal softening as temperature increase. The Helmholtz-free energies as a function of volume and temperature are derived from phonon dispersions within the quasi-harmonic approximation at six strained volumes. The calculated apparent bulk coefficients of thermal expansion of these three phases are evaluated, the highest value approximately 13.4× 10⁻⁶ K⁻¹ within a temperature range of 500–2000 K for the rutile I4₁md phase. The lattice thermal conductivity calculated by the Debye–Callaway model suggested that the rutile type I4₁md phase has the lowest value of approximately 2.1 W/m/K at 1800 K. The other two phases, C2/m and P2/c, exhibit higher values due to relatively lower Grüneisen parameters and larger phonon velocities. The melting point of CrTaO₄ is predicted to be between 1975 and 2449 K using ab initio molecular dynamics simulations. This work provides a comprehensive theoretical understanding of the thermodynamic, mechanical, and thermal properties for the new material CrTaO₄ and serves as an example of a viable computational design strategy for improved oxidation resistance of refractory alloys at high temperatures.