Remarkably enhanced dynamic oxygen migration on graphene oxide supported by copper substrate

Abstract

The dynamic covalent properties of graphene oxide (GO) are of fundamental interest to a broad range of scientific areas and technological applications. It remains a challenge to access feasible dynamic reactions for reversibly breaking/reforming the covalent bonds of oxygen functional groups on GO, although these reactions can be induced by photonic or mechanical routes, or mediated by adsorbed water. Here, using density functional theory calculations, we demonstrate the remarkably enhanced dynamic oxygen migration along the basal plane of GO supported by copper substrate (GO@copper), with C–O bond breaking reactions and proton transfer between neighboring epoxy and hydroxyl groups. Compared to reactions on GO, the energy barriers of oxygen migrations on GO@copper are sharply reduced to be less than or comparable to thermal fluctuations, and meanwhile the crystallographic match between GO and copper substrate induces new oxygen migration paths on GO@copper. This work sheds light on understanding of the metal substrate-enhanced dynamic properties of GO, and evidences the strategy to tune the activity of two-dimensional-interfacial oxygen groups for various potential applications.