Low-Temperature Fabrication and Structure–Property Correlation in Ion-Conductive ZrO2–Y2O3–SiO2–Li2O Glass-Ceramics

Conventional ceramics often require energy-intensive, high-temperature processing, which constrains their sustainability. Herein, we report an ionic melt-induced liquid-phase-assisted process to synthesize ZrO2–Y2O3–SiO2–Li2O glass-ceramics, reducing typical processing temperatures by ∼400 °C without cold isostatic pressing. By leveraging ZrO2–Y2O3 as the primary network former and SiO2–Li2O as an ionic flux, we achieve tailored glass transition (Tg = 866 °C) and crystallization (Tc = 1066 °C) temperatures. This enables low-temperature crystallization while enhancing the ionic conductivity. Phase analysis confirms coexisting tetragonal and monoclinic ZrO2, Li2SiO3, and residual SiO2–Li2O glass, with minimal nonbridging oxygen content contributing to optimized mechanical properties. The optimal composition (ZrO2–Y2O3:SiO2–Li2O = 1:1.14, molar ratio) delivers exceptional Vickers hardness (8.25 GPa), Young’s modulus (109.2 GPa), and ionic conductivity. This work outlines a sustainable pathway for the development of advanced glass-ceramics and solid electrolytes with potential implications for structural materials, functional devices, and solid-state batteries.