Biomimetic Architectured Graphene Aerogel with Exceptional Strength and Resilience

Materials combining lightweight, robust mechanical performances, and multifunctionality are highly desirable for engineering applications. Graphene aerogels have emerged as attractive candidates. Despite recent progresses, the bottleneck remains how to simultaneously achieve both strength and resilience. While multiscale architecture designs may offer a possible route, the difficulty lies in the lack of design guidelines and how to experimentally achieve the necessary structure control over multiple length scales. The latter is even more challenging when manufacturing scalability is taken into account. The Thalia dealbata stem is a naturally porous material that is lightweight, strong, and resilient, owing to its architecture with three-dimensional (3D) interconnected lamellar layers. Inspired by such, we assemble graphene oxide (GO) sheets into a similar architecture using a bidirectional freezing technique. Subsequent freeze-drying and thermal reduction results in graphene aerogels with highly tunable 3D architectures, consequently an unusual combination of strength and resilience. With their additional electrical conductivity, these graphene aerogels are potentially useful for mechanically switchable electronics. Beyond such, our study establishes bidirectional freezing as a general method to achieve multiscale architectural control in a scalable manner that can be extended to many other material systems.