Supercompressible Coaxial Carbon Nanotube@Graphene Arrays with Invariant Viscoelasticity over −100 to 500 °C in Ambient Air

Vertically aligned carbon nanotube (CNT) arrays have been recognized as promising cushion materials because of their superior thermal stability, remarkable compressibility, and viscoelastic characteristics. However, most of the previously reported CNT arrays still suffer from permanent shape deformation at only moderate compressive strains, which considerably restricts their practical applications. Here, we demonstrate a facile strategy of fabricating supercompressible coaxial CNT@graphene (CNT@Gr) arrays by using a two-step route involving encapsulating polymer layers onto plastic CNT arrays and subsequent annealing processes. Notably, the resulting CNT@Gr arrays are able to almost completely recover from compression at a strain of up to 80% and retain ∼80% recovery even after 1000 compression cycles at a 60% strain, demonstrating their excellent compressibility. Furthermore, they possess outstanding strain- and frequency-dependent viscoelastic responses, with storage modulus and damping ratio of up to ∼6.5 MPa and ∼0.19, respectively, which are nearly constant over an exceptionally broad temperature range of −100 to 500 °C in ambient air. These supercompressibility and temperature-invariant viscoelasticity together with facile fabrication process of the CNT@Gr arrays enable their promising multifunctional applications such as energy absorbers, mechanical sensors, and heat exchangers, even in extreme environments.