Abstract

High hardness is desirable for thermal insulation materials in various applications to improve wear resistance. However, hard materials like diamond, Si3N4, and SiC are often accompanied by high thermal conductivity, due to their strong covalent bonds and high Young’s modulus, which increase sound velocity and benefit heat transportation. How to achieve concurrent high hardness and low thermal conductivity remains a challenge in thermal insulation materials. In this work, we report (Yb+Ca) co-doped α-SiAlON (Yb0.5Ca0.75Si7.5Al4.5O1.5N14.5, a solid solution of α-Si3N4) with a low thermal conductivity of 3.4 W/(m·K) and a hardness of 18.1 GPa at 25℃. The thermal conductivity of α-SiAlONs co-doped by (Yb+Nd/Lu) were also studied, and we found that phonon scattering could be significantly increased only when there was a remarkable difference in cation mass and radius between the co-doping cations, like that between Yb3+ and Ca2+. Additionally, high-entropy α-SiAlONs co-doped by five kinds of cations were studied (e.g., Nd0.1Gd0.1Dy0.1Er0.1Yb0.1Si9.5Al2.5ON15), and we found that the high-entropy strategy is not so effective in pursuing low thermal conductivity in α-SiAlONs. The contribution of different phonon scattering mechanisms in the α-SiAlONs was discussed based on inverse thermal diffusivity. Compared with most other ceramics (e.g., 8YSZ and rare-metal zirconates) with low thermal conductivity, (Yb+Ca) co-doped α-SiAlON has a lower bulk density, higher hardness, and higher toughness, which makes it a potential candidate material for applications requiring both thermal insulation and good mechanical properties.

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