▎ 摘　　要

In this work, the role of surface oxygen in the early stage of graphene growth is investigated using density functional theory (DFT) and first-principles molecular dynamics (FPMD) simulation. For the complete dehydrogenation of CH4 on a bare or oxygen-pre-adsorbed Cu(1 1 1) surface, reaction pathways and energy barriers are compared using the Climbing Image Nudged Elastic Band method (CI-NEB). Then, the dynamics of surface oxygen with regard to graphene growth is discussed by analyzing the behavior of CH fragments on an oxygenpre-adsorbed Cu(1 1 1) surface for two different temperatures using FPMD. After analyzing the effect of oxygen on carbon feedstock dissociation and aggregation in the context of graphene growth, it can be concluded that surface oxygen is a decisive factor during oxidation, dehydrogenation, and carbon movement. It facilitates both reduced graphene nucleation density and film coverage, as well as a high growth rate for graphene.