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A graphyne (GY) family composed of the triple (sp) and double (sp2)bonds-hybridized carbon atoms is a promising allotrope of carbon for thedevelopment of nanoscale electronic devices. Unlike graphene, the GY familycontaining carbon sp bonds remains an unsolved problem in efficienttwo-dimensional (2D) growth due to monomer instability and side reactions.Herein, we synthesize GY into a single 2D layer by chemical vapor deposition(CVD) at low temperatures preventing unexpected reactions, using1,3,5-tribromo-2,4,6-triethynylbenzene (TBTEB). The CVD-grown GY via asurface-confined coupling between TBTEB monomers on a copper surface can be ridof either one-dimensional (1D) or three-dimensional (3D) growths via sidereactions. The CVD-grown GY exhibits a hexagonal lattice structure containing asingle sp-carbon bond in a link between two adjacent hexagons, consisting withthe structure of gamma-GY. This work opens a new avenue for synthesizinglarge-scale and single-crystalline GY that can be capable of versatileapplications with theoretically expected properties.

Few-Layered Graphyne Growth by an On-Surface Coupling Reaction via Alkynyl Vapour Deposition