Catalyst‐Free Synthesis of Few‐Layer Graphdiyne Using a Microwave‐Induced Temperature Gradient at a Solid/Liquid Interface

Abstract

Graphdiyne (GDY), a 2D carbon allotrope, is predicted to possess high carrier mobility and an intrinsic bandgap. However, the controlled synthesis of mono‐ or few‐layer GDY with good crystallinity remains challenging because of the instability of the monomers. Herein, a rapid and catalyst‐free synthetic method is presented for few‐layer GDY involving the use of a solid/liquid interface and a microwave‐induced temperature gradient. Sodium chloride, which can absorb microwave energy, is used as the solid substrate in a nonabsorbing solvent. A temperature gradient is formed at the solid/liquid interface under microwave irradiation, facilitating the cross‐coupling reaction of monomers at the solid surface and stabilizing the monomers in the bulk solution. Few‐layer GDY with an average thickness of less than 2 nm, a field‐effect mobility of 50.1 cm2 V−1 s−1, and p‐type characteristics is successfully obtained. This wet chemical approach may be extended to the synthesis of other few‐layered 2D materials with improved quality.

Graphdiyne‐Supported Atomic Catalysts: Synthesis and Applications

“…Recently, few-layered GDY was synthesized via a microwave-induced temperature gradient method at the solid/liquid interface. [41] NaCl was chosen as the microwave absorbing solid while the HEB dissolving in a mixture of toluene and hexane consisted of the non-absorbing system. When irradiated by microwaves, the NaCl would be heated and the solution would remain unheated, a temperature gradient will form at the solid/liquid interface (Figure 4d).…”

“…Reproduced from reference [40] with permission from Wiley‐VCH; c) CVD method for monolayered GDY [38] . Reproduced from reference [38] with permission from Wiley‐VCH; d) Microwave‐induced temperature gradient method for few‐layered GDY synthesis [41] . Reproduced from reference [41] with permission from Wiley‐VCH.…”

“…Inorganic salts‐lithium hexafluorosilicate (Li 2 SiF 6 ) was utilized wherein the anion had a strong interaction with GDY and the cation diffused into the interlayers (Figure 4b). Recently, few‐layered GDY was synthesized via a microwave‐induced temperature gradient method at the solid/liquid interface [41] . NaCl was chosen as the microwave absorbing solid while the HEB dissolving in a mixture of toluene and hexane consisted of the non‐absorbing system.…”

“…[38] Reproduced from reference [38] with permission from Wiley-VCH; d) Microwave-induced temperature gradient method for few-layered GDY synthesis. [41] Reproduced from reference [41] with permission from Wiley-VCH.…”

Graphdiyne: from Preparation to Biomedical Applications

“…Confined synthesis strategy uses strategies, such as concentration diffusion, template effect, interface restriction or temperature gradient to limit the target substrate or react in a certain space, which can prepare 2D materials. These confined strategies can deal with the poor stability of the monomer, the lower reaction efficiency and side reactions, and also the single bond between the diacetylenefree rotation [37,44,45] . Fig.…”