Graphene
is well-known as one of the best solid lubricants for
its superlubricity and high mechanical strength. Weak adhesion leading
to low interfacial compatibility is a significant challenge of the
use of graphene in harsh conditions. In this work, guided by density
functional theory (DFT) calculations, we propose a method to improve
graphene compatibility on Fe2O3 by substituting
B, P, S, and Si to some carbon sites. The results of binding energy
and potential energy surface (PES) show that the selection of suitable
elements with a reasonable concentration not only greatly improves
graphene adhesion but also provides a better frictional property than
that with pure graphene. The doped-graphene chemically binds on the
surface through the formation of covalent bonds between the dopant
atoms and iron of the surface. Bader charge analyses suggest that
the doping of B and P causes a severe charge alteration at the nearest
carbon C1, and a strong repulsion at the C1–C1 stacking sites
at the sliding interface, leading to a reduction in corrugation energies
and thus nanoscale friction. Furthermore, first-principles molecular
dynamics (FPMD) simulations at high temperature reveal that thanks
to well-adhered behavior, the doped-graphene shows a significant reduction
in the structural deformation, especially the out-of-plane component,
which is essential to maintain graphene’s ultralow friction
regime under harsh conditions. The current results shed light on further
improved graphene performance without affecting its superlubricity.