| Abstract: | It is essential to understand the size scaling effects on the mechanical properties of graphene networks to realize the potential mechanical applications of graphene assemblies. Here, a “highly dense‐yet‐nanoporous graphene monolith (HPGM)” is used as a model material of graphene networks to investigate the dependence of mechanical properties on the intrinsic interplanar interactions and the extrinsic specimen size effects. The interactions between graphene sheets could be enhanced by heat treatment and the plastic HPGM is transformed into a highly elastic network. A strong size effect is revealed by in situ compression of micro‐ and nanopillars inside electron microscopes. Both the modulus and strength are drastically increased as the specimen size reduces to ≈100 nm, because of the reduced weak links in a small volume. Molecular dynamics simulations reveal the deformation mechanism involving slip‐stick sliding, bending, buckling of graphene sheets, collapsing, and densification of graphene cells. In addition, a size‐dependent brittle‐to‐ductile transition of the HPGM nanopillars is discovered and understood by the competition between volumetric deformation energy and critical dilation energy. |
