▎ 摘　　要

As one type of versatile functional composites, graphene-embedded metal matrix, particularly for the nickel metal, has received much attention due to the mechanical enhancement effect. For the promising graphenenickel composite (Gr-Ni), one of major challenges is the intrinsically weak interfaces that leads to undesired mechanical failure. To address this issue, some structural modifications are highly required for re-designing the interface towards mechanical robustness. In this work, cationic substitution for nickel and anionic replacement for graphene are rationally adopted to modify the Gr-Ni interface from a theoretical perspective. It is expected that these modifications could induce electronic coupling and/or chemical bonding effects. Specifically, a series of transition metal atoms, including chromium, manganese, iron, cobalt, and copper, are selected for the partial substitution of nickel matrix, and meanwhile the anionic boron is introduced into graphene framework. By systematic evaluation on the properties of the Gr-Ni interface, it is evidenced that the chromium-substituted nickel matrix delivers the strongest adsorption capability towards the boron-doped graphene. Furthermore, the atomic arrangement states and the substitution concentrations are explored for optimizing binding abilities. These theoretical calculation results shed light on the interfacial enhancement strategy by the effective modulation on the atomic composition over metal-graphene interfaces and offer useful guidelines on the experimental manipulation on mechanically reinforced metal-graphene composites.