Hydrosilylation Adducts to Produce Wide‐Temperature Flexible Polysiloxane Aerogel under Ambient Temperature and Pressure Drying

Despite incorporation of organic groups into silica‐based aerogels to enhance their mechanical flexibility, the wide temperature reliability of the modified silicone aerogel is inevitably degraded. Therefore, facile synthesis of soft silicone aerogels with wide‐temperature stability remains challenging. Herein, novel silicone aerogels containing a high content of Si are reported by using polydimethylvinylsiloxane (PDMVS), a hydrosilylation adduct with water‐repellent groups, as a “flexible chain segment” embedded within the aerogel network. The poly(2‐dimethoxymethylsilyl)ethylmethylvinylsiloxane (PDEMSEMVS) aerogel is fabricated through a cost‐effective ambient temperature/pressure drying process. The optimized aerogel exhibits exceptional performance, such as ultra‐low density (50 mg cm−3), wide‐temperature mechanical flexibility, and super‐hydrophobicity, in comparison to the previous polysiloxane aerogels. A significant reduction in the density of these aerogels is achieved while maintaining a high crosslinking density by synthesizing gel networks with well‐defined macromolecules through hydrolytic polycondensation crosslinking of PDEMSEMVS. Notably, the pore/nanoparticle size of aerogels can be fine‐tuned by optimizing the gel solvent type. The as‐prepared silicone aerogels demonstrate selective absorption, efficient oil–water separation, and excellent thermal insulation properties, showing promising applications in oil/water separation and thermal protection. A soft polysiloxane aerogel is designed and successfully fabricated through the condensation process of polydimethylvinylsiloxane macromolecules. In addition to its ultra‐lightweight nature, this material possesses several advantageous properties, including exceptional mechanical stability when exposed to liquid nitrogen, effective thermal insulation, super‐hydrophobicity, and notable advancements in porous material development.