Graphene oxide nanosheets augment silk fibroin aerogels for enhanced water stability and oil adsorption.

Nanocomposite aerogels exhibit high porosity and large interfacial surface areas, enabling enhanced chemical transport and reactivity. Such mesoporous architectures can be prepared by freeze-casting naturally-derived biopolymers such as silk fibroin, but often form mechanically weak structures that degrade in water, which limits their performance under ambient conditions. Adding 2D material fillers such as graphene oxide (GO) or transition metal carbides ( e.g. MXene) could potentially reinforce these aerogels via stronger intermolecular interactions with the polymeric binder. Here, we show that freeze-casting of GO nanosheets with silk fibroin results in a highly water-stable, mechanically robust aerogel, with considerably enhanced properties relative to silk-only or silk-MXene aerogels. These silk-GO aerogels exhibit high contact angles with water and are highly water stable. Moreover, aerogels can adsorb up 25-35 times their mass in oil, and can be used robustly for selective oil separation from water. This increased stability may occur due to strengthened intermolecular interactions such as hydrogen bonding, despite the random coil and α-helix conformation of silk fibroin, which is typically more soluble in water. Finally, we show these aerogels can be prepared at scale by freeze-casting on a copper mesh. Ultimately, we envision that these multicomponent aerogels could be widely utilized for molecular separations and environmental sensing, as well as for thermal insulation and electrical conductivity.