Influence of Graphene Reduction and Polymer Crosslinking on Improving Interfacial Properties of Multilayer Thin Films

Graphene is a versatile composite reinforcement candidate due to its strong mechanical, tunable electrical and optical properties, and chemical stability. However, one drawback is the weak interfacial bonding, which results in weak adhesion to substrates. This could be overcome by adding polymer layers to have stronger adherence to the substrate and between graphene sheets. These multilayer thin films were found to have lower resistance to lateral scratch forces when compared to other reinforcements such as polymer/clay nanocomposites. Two additional processing steps are suggested to improve the scratch resistance of these films: graphene reduction and polymer cross-linking. Graphene/polymer nanocomposites consisting of polyvinylamine (PVAm) and graphene oxide (GO) were fabricated using the layer-by-layer assembly (LbL) technique. The reduced elastic modulus and hardness of PVAm/GO films were measured using nanoindentation. Reducing GO enhances mechanical properties by 60–70% while polymer cross-linking maintains this enhancement. Both graphene reduction and polymer cross-linking show significant improvement to scratch resistance. Particularly, polymer cross-linking leads to films with higher elastic recovery, 50% lower adhesive and plowing friction coefficient, 140 and 50% higher adhesive and shear strength values, respectively, and lower material pileup and scratch width/depth.