Engineering the interface in mechanically responsive graphene-based films

Due to their extraordinary mechanical properties, nanocarbon materials (e.g. carbon nanotube and graphene) are attracting great interests in the field of nanocomposites. One unique feature in nanocarbon-based nanocomposites is their intrinsically rich interface, allowing them to adapt the microstructures in response to external loading and, in turn, to stiffen themselves. This mechanical behavior, called responsive stiffening, was usually observed in biological materials such as bones and muscles. The mechanically responsive behaviors of nanocarbon-based materials are particularly exciting because the nanocarbon-enabled huge interface area offers opportunities to tune such stiffening performance while this interface advantage is not fully exploited yet. Here, we demonstrate stiffening behaviors in graphene oxide (GO)-based film materials in response to dynamic oscillations. Through a facile method of polymer content alteration and alkali treatment, the microstructure and interlayer interaction of GO films are modified, along with the resulted responsively stiffening performance. Based on polarized Raman spectra characterizations, we attribute the stiffening mechanism to the microstructural evolution of GO films during dynamic tension as well as the polymer chains alignment. Finally, we highlight the significantly improved static mechanical properties of GO film after a simple stiffening process. Our results not only aid in the development of biomimetic, adaptive materials, but provide a mechanical way for the design of high-performance nanocarbon-based nanocomposites.