High-Performance Methylsilsesquioxane Aerogels: Hydrolysis Mechanisms and Maximizing Compression Properties

Synthesis of methylsilsesquioxane aerogels by ambient pressure drying instead of supercritical drying has recently emerged as a major trend, but the issues of low mechanical strength and unstable performance still need to be resolved. This work reveals the microscopic formation mechanisms of gel skeleton based on the kinetic characteristics of methyltrimethoxysilane (MTMS) precursor hydrolysis and the associated sol-gel reactions. The effects of oxalic acid concentration (c(OA)) and hydrolysis time of MTMS solution (t(h)) on the gelation time, morphologies, microstructures, chemical structure, and compression properties of the as-synthesized methylsilsesquioxane aerogels are investigated. The optimal c(OA) and t(h) are 38.4 mmol/L and 120 min, respectively, endowing the methylsilsesquioxane aerogels with a compression strength of 0.170 MPa and a maximum compression strain of 61.2%. Precise control of the hydrolysis conditions ensures the formation of branched particle-to-particle networks, which is crucial for maximizing the compression properties of methylsilsesquioxane aerogels synthesized under industry-relevant conditions.