Mechanically Reinforced Silica Aerogels via Thermally Induced Phase Separation of Poly(ethylene-co-vinyl Alcohol)

Silica aerogels are highly attractive due to their outstanding properties, including their low density, ultralow thermal conductivity, large porosity, high optical transparency, and strong sorption activity. However, their inherent brittleness has limited widespread applications. Constructing a robust, highly porous three-dimensional network is critical to achieving the desired mechanical properties in aerogels. In this study, we introduce a novel synthesis route for fabricating lightweight and mechanically strong aerogels by incorporating poly(ethylene-co-vinyl alcohol) (EVOH) through thermally induced phase separation (TIPS). EVOH exhibits upper critical solution temperature (UCST) behavior in a mixture of isopropanol (IPA) and water, which can be utilized to reinforce the silica skeletal structure. Robust aerogels were prepared via the sol-gel process and TIPS method, followed by supercritical CO₂ drying, yielding samples with bulk densities ranging from 0.136 to 0.200 g/cm³. N₂ physisorption analysis revealed a mesoporous structure, with the specific surface area decreasing from 874 to 401 m²/g as EVOH content increased from 0 to 80 mg/mL. The introduced EVOH significantly enhanced mechanical performance, raising the flexural strength and compressive strength to 0.545 MPa and 18.37 MPa, respectively-far exceeding those of pure silica aerogel (0.098 MPa and 0.74 MPa). This work demonstrates the effectiveness of the TIPS strategy for developing high-strength, low-density silica aerogels with well-preserved porosity.