Large‐Scale Synthesis of Few‐Layered Graphene using CVD

Large‐scale, substrate‐free graphene, with few‐layered sheets, is synthesized by the CVD of methane over cobalt supported on magnesium oxides at 1000 °C in a gas flow of argon. Typically, 50 mg of the few‐layered graphene materials over 500 mg of the Co/MgO catalysts are synthesized under our experimental conditions. Randomly aggregated, thin, crumpled graphene sheets stacked closely together are produced. Both carbon (94.6 at.‐%) and oxygen (5.4 at.‐%) are present in the graphene sheets. The oxygen may originate from air adsorbed on the graphene sheets. Our results indicate the presence of localized sp 3 defects within the sp 2 carbon network and small sp 2 domains in the few‐layered graphene particles.