Environmental barrier coatings (EBCs) are widely used to protect ceramic matrix composites (CMCs, SiCf/SiC, and Al2O3f/Al2O3), and they should have low thermal expansion coefficients (TECs) matching the CMCs and excellent mechanical properties to prolong their lifetime. Current EBC materials have disadvantages of phase transitions and insufficient mechanical properties, which affect their working temperatures and lifetime. It is necessary to develop new oxide EBCs. Ytterbium tantalate (YbTaO4) is a stable and novel EBC material, and we have improved the mechanical properties and TECs of Yb1−xAlxTaO4 (x = 0.05, 0.1, 0.2, 0.3, 0.4, 0.5) ceramics by replacing Yb with Al. XRD, SEM, and EDS are used to verify the crystal and microstructures, and nano-indentation is used to measure the modulus and hardness when changes in TECs are measured within a thermal expansion device. The results show that the phase structure of Yb1−xAlxTaO4 (x = 0.05, 0.1, 0.2, 0.3, 0.4, 0.5) is stable at 25–1400 °C within air atmosphere, and their high-temperature TECs (6.4–8.9 × 10−6 K−1, 1400 °C) are effectively regulated by introductions of different contents of Al, which enlarge their engineering applications for SiCf/SiC and Al2O3f/Al2O3 CMCs. The evolutions of TECs are analyzed from structural characteristics and phase compositions, and the increased TECs make Yb1−xAlxTaO4 potential EBCs for Al2O3 matrixes. Due to the high bonding strength of Al–O bonds, hardness, as well as Young’s modulus, are enhanced with the increasing Al content, with Yb1−xAlxTaO4 (x = 0.05, 0.1, 0.2, 0.3, 0.4, 0.5) having a nano-hardness of 3.7–12.8 GPa and a Young’s modulus of 100.9–236.6 GPa. The TECs of YbTaO4 are successfully regulated to expand their applications, and they match those of Al2O3 and SiC matrixes, as well as displaying improved mechanical properties. This work promotes applications of YbTaO4 as potential EBCs and provides a new way to regulate the TECs of tantalates.
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