SmTaO4, Sm3TaO7 and SmTa3O9 ceramics were prepared via a high temperature solid-state reaction. The results show that the phase structures of the SmTaO4 ceramics are a monoclinic phase (space group: I2 (5)), the Sm3TaO7 ceramics are an ordered orthorhombic phase (space group: Ccmm), and the SmTa3O9 ceramics are an orthorhombic phase (space group: Cmmm). Macromolecular and crystal structures of Sm3TaO7 and SmTa3O9 are more complex than those of SmTaO4, which can enhance phonon scattering and reduce thermal conductivity. Compared with those of SmTaO4 and SmTa3O9, Sm3TaO7 has the smallest grain size, indicating that a small grain size has an effect on strength and ensures material stability. Because of a distorted TaO6 octahedron and a high concentration of cation vacancy in the lattice of SmTa3O9, its thermal conductivity increases with increasing temperature. Compared with that of 7–8 YSZ, Sm3TaO7 has a low thermal conductivity (1.3–1.7 W·m−1·K−1 at 100 °C–900 °C), and its minimum thermal conductivity is nearly 30% lower than that of YSZ. The Sm3TaO7 ceramics have the highest TECs at approximately 9.82 × 10−6 K−1 at 1200 °C, which is close to that of 7–8 YSZ (approximately 10 × 10−6). This indicates that Sm3TaO7 has the potential to be employed as a thermal barrier coating.
SmTaO4 ceramics have excellent high-temperature phase stabilities and mechanical properties and show great potential for use as next-generation thermal barrier coating (TBC) materials. CeO2–SmTaO4 ceramics are prepared via high-temperature solid–state reaction. It retains a single monoclinic phase structure. Ce4+ was reduced to Ce3+ by high-temperature deoxidation, and the Ce3+ ions substitute for an equal number of Sm3+ ions. The CeO2–SmTaO4 ceramics had lower thermal conductivities [1.09–2.75 W/(m K)] than yttria-stabilized zirconia (YSZ) [2.1–2.7 W/(m K)] at 100–800 °C, which decreased dramatically with increasing temperature. SmTaO4 doped with 2% CeO2 had lower thermal conductivity [1.09 W/(m K), 800 °C] than SmTaO4 [1.42 W/(m K), 800 °C] and 2% ZrO2-doped SmTaO4 ceramics [1.22 W/(m K), 800 °C]. The low thermal conductivity is attributed to Ce3+ substitution for an equal number of Sm3+ ions, and because Ce3+ ions are the strongest phonon scattering centers, they can decrease the phonon mean free path effectively. The thermal expansion coefficient of 8% CeO2–SmTaO4 ceramics is approximately 10.3 × 10−6 K−1 at 1200 °C, which is slightly higher than that of both YSZ (10.0 × 10−6 K−1) and SmTaO4 (9.58 × 10−6 K−1). The outstanding thermophysical properties indicate that CeO2–SmTaO4 ceramics are potential TBC materials.