Processing and Characterization of Refractory Quaternary and Quinary High-Entropy Carbide Composite

Quaternary high-entropy ceramic (HEC) composite was synthesized from HfC, Mo₂C, TaC, and TiC in pulsed current processing. A high-entropy solid solution that contained all principal elements along with a minor amount of a Ta-rich phase was observed in the microstructure. The high entropy phase and Ta-rich phase displayed a face-centered cubic (FCC) crystal structure with similar lattice parameters, suggesting that TaC acted as a solvent carbide during phase evolution. The addition of B₄C to the quaternary carbide system induced the formation of two high-entropy solid solutions with different elemental compositions. With the increase in the number of principal elements, on the addition of B₄C, the crystal structure of the HEC phase transformed from FCC to a hexagonal structure. The study on the effect of starting particle sizes on the phase composition and properties of the HEC composites showed that reducing the size of solute carbide components HfC, Mo₂C, and TiC could effectively promote the interdiffusion process, resulting in a higher fraction of a hexagonal structured HEC phase in the material. On the other hand, tuning the particle size of solvent carbide, TaC, showed a negligible effect on the composition of the final product. However, reducing the TaC size from -325 mesh down to <1 µm resulted in an improvement of the nanohardness of the HEC composite from 21 GPa to 23 GPa. These findings suggested the possibility of forming a high-entropy ceramic phase despite the vast difference in the precursor crystal structures, provided a clearer understanding of the phase transformation process which could be applied for the designing of HEC materials.