Structure–property correlation of silicone hydrogels based on 3‐[tris(trimethylsilyloxy)silyl]propyl methacrylate monomer

We have investigated silicone‐based hydrogels highlighting the effect of silyl comonomer, method of polymerization and nature of cross‐linker on their bulk as well as surface properties. Transmission electron microscopy results showed that solution thermal polymerization mitigated phase segregation of hydrophobic siloxane components over bulk thermal polymerization. 2‐hydroxyethyl methacrylate cannot provide transparent hydrogels with 3‐[tris(trimethylsilyloxy)silyl]propyl methacrylate alone and requires equal weight percent of N, N‐dimethylacrylamide to compatibilize the comonomers to yield a silicone hydrogel network showing no microphase separation. The differentiated surface properties of silicone hydrogels containing varying amount of siloxane comonomers were also unraveled and rationally supported by surface infrared spectroscopic results. Different molecular states of water entrapped within hydrogel network were identified to understand the nature of gel‐mesh functionality. The effect of silicone pendant groups on the gel elasticity was also explored.