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In the chemical vapor deposition growth of large-area graphene polycrystalline thin films, the coalescence of randomly oriented graphene domains results in a high density of uncertain grain boundaries (GBs). The structures and properties of various GBs are highly dependent on the misorientation angles between the graphene domains, which can significantly affect the performance of the graphene films and impede their industrial applications. Graphene bicrystals with a specific type of GB can be synthesized via the controllable growth of graphene domains with a predefined lattice orientation. Although the bicrystal has been widely investigated for traditional bulk materials, no successful synthesis strategy has been presented for growing two-dimensional graphene bicrystals. In this study, we demonstrate a simple approach for growing well-aligned large-domain graphene bicrystals with a confined tilt angle of 30° on a facilely recrystallized single-crystal Cu (100) substrate. Control of the density of the GBs with a misorientation angle of 30° was realized via the controllable rapid growth of sub- centimeter graphene domains with the assistance of a cooperative catalytic surface-passivation treatment. The large-area production of graphene bicrystals consisting of the sole specific GBs with a tunable density provides a new material platform for fundamental studies and practical applications.
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