Aluminum-containing high-entropy alloys (HEAs) offer promising combinations of strength, wear resistance, and thermal stability for demanding applications. This work investigates TiCuNiSi–xAl HEAs (0.5-1.7 at.% Al) fabricated via spark plasma sintering (SPS) at 600 °C under 40 MPa, focusing on the effect of Al content on densification, porosity, and hardness. Microstructural analysis (SEM/EDS, XRD) revealed progressive refinement and improved densification (67.50% → 74.45%) with increasing Al, alongside reduced porosity (32.50% → 25.55%). Peak hardness (436.85 HV) occurred at 1.7 at.% Al, linked to the formation of well-distributed Al-rich intermetallic phases. Lower Al contents produced coarser, more porous structures with reduced hardness. Findings demonstrate that controlled Al addition enhances sinterability and hardening, though excessive intermetallic formation may induce brittleness. This study establishes a composition–microstructure–property relationship, supporting the design of Al-containing HEAs for aerospace, automotive, and biomedical applications.
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