Material design using calculation phase diagram for refractory high‐entropy ceramic matrix composites

Abstract To achieve Si‐free refractory ceramic matrix composites exposed to an oxidizing atmosphere at approximately 2000°C, a Ti–Zr–Mo ternary alloy melt‐infiltration (MI) method was developed for the production of carbon fiber‐reinforced refractory high‐entropy ceramic matrix composites (C/RHECs), with high‐entropy carbides serving as the matrix. This approach was designed using calculation phase diagrams (CALPHADs) and the calculation of thermodynamic parameters. The combination of CALPHAD and the calculation of alloy and carbon reactivity enabled the prediction of reaction and infiltration behavior into a preform comprising carbon fiber, carbon black, and transition metal carbide powders. Furthermore, C/RHECs featuring a (Ti, Zr, Hf, Nb, Ta, Nb, Mo)C matrix were experimentally fabricated through the Ti–Zr–Mo alloy MI method in accordance with the design. The arc‐wind tunnel tests on the C/RHECs conducted at approximately 2000°C revealed surfaces covered with complex oxides. The apparent oxidation rate of the C/RHECs was similar to that of Si‐containing ceramics and composites. These results indicate that complex oxides act as a barrier to oxygen diffusion toward unoxidized regions, making Si no longer essential for protecting materials from oxidation above 2000°C.