Mechanics of coordinative crosslinks in graphene nanocomposites: A first-principles study

Graphene-based nanocomposites have recently received rising interest owing to their outstanding performance. Crosslinkers, such as a divalent ion based coordinative complex, have been proved to significantly improve load transfer between adjacent graphene sheets, which subsequently defines the overall mechanical properties of the composites. In this paper, the structures and mechanical properties of both interlayer and intralayer coordinative bonds are quantified through density functional theory based first-principles calculations. The structural deformation and failure mechanism are investigated under interlayer sliding and separation loads. Extensive discussion is made by comparing coordinative bonds with other types of crosslinks such as covalent bonds, van der Waals interactions and hydrogen bonds. Moreover, the impacts from the crosslink mechanisms to overall properties of nanocomposites are projected towards the applications in high-performance multifunctional materials.