Synthesis and Properties of 2D Carbon—Graphdiyne

Abstract

Graphdiyne (GDY) is a flat material comprising sp- and sp-hybridized carbon atoms with high degrees of π conjugation that features uniformly distributed pores. It is interesting not only from a structural point of view but also from the perspective of its electronic, chemical, mechanical, and magnetic properties. We have developed an in situ homocoupling reaction of hexaethynylbenzene on Cu foil for the fabrication of large-area ordered films of graphdiyne. These films are uniform and composed of graphdiyne multilayers. The conductivity of graphdiyne films, calculated at 2.52 × 10 S m, is comparable to that of Si, suggesting excellent semiconducting properties. Through morphology-controlled syntheses, we have prepared several well-defined graphdiyne structures (e.g., nanotubes, nanowires, and nanowalls) having distinct properties. The graphdiyne nanotube arrays and graphdiyne nanowalls exhibited excellent field emission performance, higher than that of some other semiconductors such as graphite and carbon nanotubes. These structures have several promising applications, for example, as energy storage materials and as anode materials in batteries. The unique atomic arrangement and electronic structure of graphdiyne also inspired us to use it to develop highly efficient catalysts; indeed, its low reduction potential and highly conjugated electronic structure allow graphdiyne to be used as a reducing agent and stabilizer for the electroless deposition of highly dispersed and surfactant-free Pd clusters. GDY-based three-dimensional (3D) nanoarchitectures featuring well-defined porous network structures can function as highly active cathodes for H evolution. Heteroatom-doped GDY structures are excellent metal-free electrocatalysts for the oxygen reduction reaction (ORR). Its excellent electrocatalytic activity and inexpensive, convenient, and scalable preparation make GDY a promising candidate for practical and efficient energy applications; indeed, we have explored the application of GDY as a highly efficient lithium storage material and have elucidated the method through which lithium storage occurs in multilayer GDY. Lithium-ion batteries featuring GDY-based electrodes display excellent electrochemical performance, including high specific capacity, outstanding rate performance, and long cycle life. We have also explored the application of GDY in energy conversion and found that it exhibits excellent conductivity. In this Account, we summarize the relationships between the functions of graphdiyne and its well-defined nanostructures. Our results suggest that GDY is a novel 2D carbon material possessing many attractive properties. It can be designed into new nanostructures and materials across a range of compositions, sizes, shapes, and functionalities and can be applied in the fields of electronics, optics, energy, and optoelectronics.

Confined Synthesis of 2D Nanostructured Materials toward Electrocatalysis

“…Nanostructured carbons, such as 0D fullerenes,61 1D carbon nanotubes,62 and 2D graphene,63 have shown intriguing physicochemical properties due to the unique sp 2 hybrid atom structure of these carbon materials. Along with the rapid development of graphene and its derivatives, 2D carbon‐based nanomaterials have attracted tremendous research interest 64,65. Up to now, a variety of interesting 2D carbon‐based nanocomposites have been synthesized based on the confined synthesis method.…”

Interfacial Synthesis of Conjugated Crystalline 2D Fluorescent Polymer Film Containing Aggregation‐Induced Emission Unit

“…For example, Li and co‐workers reported the synthesis of fully conjugated 2D graphdiyne by using Glaser–Hay coupling reaction on the surface of copper foils, which served as dual roles of catalyst and the template . Since then, many 2D graphdiyne analogues have been synthesized by the same reaction . These 2D networks constructed with sp 2 ‐ and sp‐hybridized carbons exhibit high degrees of π conjugation, evenly distributed pores, and tunable electronic properties, showing vast potentials in catalysis, energy storage, biotechnology.…”

Interdiffusion at Room Temperature in Cu-Ni(Fe) Nanolaminates

“…Nanolaminates, functional multilayers, and their 2D unit materials are of general importance to fields such as improvements in fracture toughness for medical application [9], energy storage and battery anodes using electrochemical nanoarchitectonics [10,11], and magnetic materials with tunable in-plane anisotropy [12]. The relevance of interdiffusion in nanolaminates is of great importance regarding these applications as well as many others for assessing the robustness of structure in the context of maintaining performance over lifetime use.…”