Due to their excellent properties and two-dimensional geometry, graphenes (Grs) have been widely used as reinforced fillers in graphene/aluminum nanolaminated composite (GANC). The separation and slippage behavior of the GANC is highly dependent on the interfacial properties between Gr and aluminum (Al). In this study, two interfacial failures of GANCs, i.e., pull-up failure and pull-out failure, were investigated using a molecular dynamics (MD) method. The effects of the crystal orientation of single-crystal Al component and the geometry of the Gr component on the normal and shear interfacial properties of the GANC were examined. It was evident that the interfacial pull-up resistance resulted from the atomic forces of all the atoms at the interface, whereas the interfacial shear force during pull-out stems from the atomic forces of the atoms at the crack tip. In addition, the studies revealed that the interface bonding strength between the Gr and Al was sensitive to both the crystal orientation of the Al and the environmental temperature. Finally, the cohesive law was used to describe the interfacial behavior of the Gr and Al, providing the interfacial data for the finite element modeling of composites with Gr and Al interface.
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