Synergistic Effects of Mg₂Si-YH₂ Composite Additives on the Microstructure and Properties of Silicon Nitride Ceramics

Sintering additives play a decisive role in the densification behavior, mechanical properties, and thermal conductivity of silicon nitride ceramics. In this study, Mg₂Si and YH₂ were used as sintering additives for gas pressure sintering of silicon nitride based on the synergistic mechanism of “silicide silicon extraction-hydride dehydrogenation”. The regulation rules of the additives on ceramic densification, mechanical properties, and thermal conductivity were systematically investigated. Two optimization strategies were proposed for the technical route of replacing traditional oxide additives with non-oxide systems. (i) Rare-earth hydride YH₂ was used to replace traditional rare-earth oxides. It reacts with SiO₂ to achieve strong deoxidation and precisely regulate the liquid phase composition. (ii) Metal silicide Mg₂Si was used to replace metal oxides. It promotes the preferred growth of β-Si₃N₄ grains, consumes oxygen in the system, and reduces lattice defects. Mg₂Si introduces Si into the liquid phase, increasing the Si/O ratio, which lowers lattice oxygen content and supports higher thermal conductivity. YH₂ consumes SiO₂ on the Si₃N₄ surface, which reduces liquid phase oxygen content and inhibits lattice oxygen incorporation, promoting a liquid phase with a high N/O ratio. Compared with traditional Y₂O₃, YH₂ increases the Y₂O₃/SiO₂ ratio in the liquid phase. It promotes grain growth, reduces SiO₂ activity, and further improves the thermal conductivity of ceramics. Silicon nitride ceramics prepared by gas pressure sintering at 1750 °C with 3 wt.% Mg₂Si and 4 wt.% YH₂ composite additives exhibit the highest thermal conductivity of 87 W/(m·K), with a Vickers hardness of 14.36 GPa and a flexural strength of 643.15 MPa. This study provides an innovative idea for the preparation of high-performance silicon nitride heat dissipation substrates.