Face-to-face crosslinking of graphdiyne and related carbon sheets toward integrated graphene nanoribbon arrays

The fabrication of graphene nanoribbon (GNR) arrays in which GNRs have precise widths and edge configurations is critical for the practical application of graphene-based materials into nanoelectronics. Using density functional theory calculations, we study and establish the structural and chemical relationship for three well-known carbon nanostructures: GNRs, graphdiyne and related carbon sheets, and carbon honeycomb frameworks (CHFs). Graphdiyne and related carbon sheets containing CC triple bonds can be chemically converted into the corresponding CHFs through the face-to-face crosslinking reactions of their triple bonds. The yielded CHFs are thermodynamically stable and intrinsically incorporate orderly-aligned GNR arrays. The incorporated GNRs have either armchair or zigzag edges, depending on the A- or Z-type crosslinking reactions the carbon sheets undergo. CHFs incorporating zigzag edged GNRs can have ferromagnetic ground states with unpaired electrons located at the zigzag edges. The edges of CHFs derived from graphdiyne-like carbon sheets, including unpaired electrons localized at zigzag edges, are chemically inert against O2 and H2 passivation. Therefore, the face-to-face crosslinking reactions of graphdiyne and related carbon sheets may serve as a promising way to design and synthesize 3D carbon architectures that integrate orderly-aligned and edge-protected GNR arrays with atomically precise structures.

250