Enhanced interlayer adhesion of wetted graphene oxide by confined water bridge

Graphene oxide (GO) sheets are widely used as building blocks in flexible electronic devices, structural materials, and energy storage technology owing to physicochemical flexibility and remarkable mechanical properties. GO exists as lamellar structures in these applications and, thus, it urges to enhance interface interaction to prevent interfacial failure. This study explores the adhesion of GO with and without intercalated water utilizing steered molecular dynamics (SMD) simulations. We find the interfacial adhesion energy (γ) depends on the synergistic effect of the types of functional groups, the degree of oxidation (c), and water content (wt). The intercalated monolayer water confined within GO flakes can improve the γ by more than 50% whereas the interlayer spacing is enlarged. The enhancement of adhesion is from the cooperative hydrogen bonding bridges between confined water and functional group on GO. Furthermore, the optimal water content wt = 20% and oxidation degree c = 20% are obtained. Our findings provide an experimentally available way to improve interlayer adhesion through molecular intercalation, which opens the possibility of high-performance laminate nanomaterial-based films for versatile applications.