Multifunctional Superelastic Cellulose Nanofibrils Aerogel by Dual Ice‐Templating Assembly

Many applications proposed for graphene require multiple sheets be assembled into a monolithic structure. The ability to maintain structural integrity upon large deformation is essential to ensure a macroscopic material which functions reliably. However, it has remained a great challenge to achieve high elasticity in three-dimensional graphene networks. Here we report that the marriage of graphene chemistry with ice physics can lead to the formation of ultralight and superelastic graphene-based cellular monoliths. Mimicking the hierarchical structure of natural cork, the resulting materials can sustain their structural integrity under a load of >50,000 times their own weight and can rapidly recover from >80% compression. The unique biomimetic hierarchical structure also provides this new class of elastomers with exceptionally high energy absorption capability and good electrical conductivity. The successful synthesis of such fascinating materials paves the way to explore the application of graphene in a self-supporting, structurally adaptive and 3D macroscopic form.

Three-dimensional nanofibrous aerogels (NFAs) that are both highly compressible and resilient would have broad technological implications for areas ranging from electrical devices and bioengineering to damping materials; however, creating such NFAs has proven extremely challenging. Here we report a novel strategy to create fibrous, isotropically bonded elastic reconstructed (FIBER) NFAs with a hierarchical cellular structure and superelasticity by combining electrospun nanofibres and the fibrous freeze-shaping technique. Our approach causes the intrinsically lamellar deposited electrospun nanofibres to assemble into elastic bulk aerogels with tunable densities and desirable shapes on a large scale. The resulting FIBER NFAs exhibit densities of >0.12 mg cm(-3), rapid recovery from deformation, efficient energy absorption and multifunctionality in terms of the combination of thermal insulation, sound absorption, emulsion separation and elasticity-responsive electric conduction. The successful synthesis of such fascinating materials may provide new insights into the design and development of multifunctional NFAs for various applications.