Tunable Interlayer Interactions in Reduced Graphene Oxide Paper

Free-standing graphene-based paper-like materials have garnered significant interest for various applications because of their tunable physical and chemical properties, along with unique multilayered structures. Because of the layered configuration of graphene paper, characterization of the interactions between graphene sheets is critical for understanding its fundamental properties and applications. We investigate the interlayer cohesion energies in graphene papers using the mode I fracture concept with double cantilever beam specimens. Mechanical separation along the middle of the graphene paper thickness enables the evaluation of interlayer bonding strength in the paper. Starting from graphene oxide paper, the chemical reduction using hydroiodic acid tunes the interlayer cohesion energy from 11.30 ± 0.25 to 4.78 ± 0.18 J/m² as the reduction time increases. The interlayer cohesion energy is correlated with the oxygen content, interlayer spacing, and electrical conductivity of graphene papers. This work provides a fundamental characterization of the interlayer cohesion energy of graphene paper and establishes the potential for tunability of the interlayer interactions in graphene paper.