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

Abstract

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.