Mussel-Inspired Graphene Film with Enhanced Durability as a Macroscale Solid Lubricant

Graphene has exhibited massive potential as a macroscale solid lubricant, but its durability is limited due to the weak adhesion between graphene sheets and the substrate. Here, inspired by mussel adhesive protein (MAP), effective reinforcement of the graphene–substrate interaction to attain remarkable enhancement on the durability of the graphene film is presented. The mussel-inspired graphene (mGr) film exhibits a coefficient of friction stabilizing at 0.16 up to 490000 sliding cycles in the friction testing against the silicon nitride ball; in the identical sliding condition, comparatively, the graphene (Gr) film without MAP only lasts 4300 sliding cycles. The analysis of Raman and ATR-FTIR demonstrates that, on the one hand, the MAP film firmly adsorbs onto the substrate via forming metal-catechol coordination bonds with metal atoms; on the other hand, it establishes strong interactions with graphene sheets by hydrogen bonding as well as the π–π overlap. As an interlayer, MAP retains graphene sheets within the contact interface in the form of a compact tribo-layer, which results in an over 2 orders of magnitude enhancement of durability for the mGr film. This strategy of improving the graphene–substrate adhesion via MAP offers an avenue for the development of effective and reliable graphene-based solid lubricants for engineering applications.