▎ 摘　　要

The controlled growth of high-quality graphene on a large scale is of central importance for applications in electronics and optoelectronics. To minimize the adverse impacts of grain boundaries in large-area polycrystalline graphene, the synthesis of large single crystals of monolayer graphene is one of the key challenges for graphene production. Here, we develop a facile surface engineering method to grow large single-crystalline monolayer graphene by the passivation of the active sites and the control of graphene nucleation on copper surface using the melamine pretreatment. Centimeter-sized hexagonal single-crystal graphene domains were successfully grown, which exhibit ultrahigh carrier mobilities exceeding 25 000 cm2 17-1 s-1 and quantum Hall effects on SiO2 substrates. The underlying mechanism of melamine pretreatments were systematically investigated through elemental analyses of copper surface in the growth process of large single-crystals. This present work provides a surface design of a catalytic substrate for the controlled growth of large-area graphene single crystals.