Three-dimensional (3D) graphene-based porous materials with a combination of low density, superelasticity, excellent mechanical resilience and tunable functionalities can be used in diverse applications. Here we report an approach of fabricating the stable and flexible 3D graphene aerogel materials with tunable functionality via a general silane-assisted processing that maintains an effective control of the chemistry, architecture and functionality of these porous structures. Simultaneous reduction and functionalization were achieved under both a low temperature and a low graphene oxide concentration in aqueous solution via using a facile one-step co-assembly method. The introduction of silane bonding tailors both the porous microstructure and the surface property of the lightweight aerogel effectively, subsequently providing improved mechanical properties and versatile functionalities including super compressive elasticity, outstanding cyclic resilient property, good electrical conductivity, stable viscoelastic properties, high level energy absorption capacity, excellent hydrophobicity, remarkable thermal stability and extremely high sensitivity of elasticity-dependent electrical conductivity. This opens up scalable and low-cost ways to the integration of microscopic two-dimensional graphene sheets into macroscopic 3D graphene aerogel materials, thus providing the possibility of fabricating novel lightweight porous aerogel materials with controllable functionalities and reversible compressibility for applications in numerous fields.
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