Effect of strain on the reactivity of graphene films

[Display omitted] •Compressive and expansive strain increase binding energies on graphene.•Bidentate adsorbates are more strongly stabilized than monodentate or physisorbed species.•Strain improves the oxygen reduction activity of graphene and can change the dominant reaction mechanism. The effect of strain on the adsorption of atomic species (Cl, H, N, and O) on pristine and nitrogen-doped graphene is studied using density functional theory. Expansive strain increases surface reactivity by destabilizing graphene π orbitals, which is similar to the shift in the d-band center observed on stretched metal surfaces. However, compressive strain leads to the formation of nanoripples that strongly bind atomic species at ridge sites, which is fundamentally different from adsorption on compressed metal surfaces. Our findings suggest that strain can be used as an effective means of manipulating graphene’s reactivity, which is explicitly shown here for the oxygen reduction reaction.