Macroscale superlubricity breakdown

Macroscale superlubricity breakdown of lubricating materials caused by substrate surface roughening and mechanochemical modification poses great challenges for their practical tribological applications. Here, a facile way is reported to access robust macroscale superlubricity in a vacuum environment, via the operando formation of graphene/transition-metal dichalcogenide (TMDC) heterostructures at wear-induced rough surfaces. By trapping active amorphous carbon (a-C) wear products between TMDC flakes, the sandwich structures readily transform into graphene/TMDC heterostructures during running-in stage, based on shear-induced confinement and load-driven graphitization effects. Then they assemble into multipoint flake-like tribofilms to achieve macroscale superlubricity at steady stage by reducing contact area, eliminating strong cross-interface carbon–carbon interactions and polishing a-C rough nascent surface. Atomistic simulations reveal the preferential formation of graphene/TMDC heterostructures during running-in stage and demonstrate the superlubric sliding of TMDCs on the graphene. The findings are of importance to achieve robust superlubricity and provide a good strategy for the synthesis of other van der Waals heterostructures.