Mechanically Robust, Hydrophobic, and Recyclable Dynamic Aerogels via Organic–Inorganic Hybridization

Polyimine aerogels, composed of covalent adaptive networks enriched with dynamic imine bonds, have shown remarkable recycling and reprogramming capabilities, marking a notable advancement in the field. However, these aerogels are challenged by inherent hydrophilicity and difficulties in achieving homogeneous nanostructures. Here, we synthesized a series of siloxane (Si)-based polyimine aerogels (Si-DPAs) with a pearl necklace-like microstructure using readily available commercial monomers and an ambient pressure synthesis method. The resultant lightweight Si-DPAs exhibit high flexibility, crimpability, and a high degree of compressibility (up to 80% strain) with a water contact angle of 136°. Moreover, Si-DPAs exhibit chemical degradability and diverse recyclability. They can be promptly employed to fabricate homogeneous films, dynamic aerogels, and recovered adhesives (with a lap shear strength of 4.0 MPa). Additionally, they demonstrate high-value applications in oil–water separation and thermal insulation. This work underscores the potential for the scalable production of polyimine aerogels and suggests avenues for broadening their application spectrum.