Atomic-Level Functionalized Graphdiyne for Electrocatalysis Applications

Abstract

Graphdiyne (GDY) is a two-dimensional (2D) electron-rich full-carbon planar material composed of sp2- and sp-hybridized carbon atoms, which features highly conjugated structures, uniformly distributed pores, tunable electronic characteristics and high specific surface areas. The synthesis strategy of GDY by facile coupling reactions under mild conditions provides more convenience for the functional modification of GDY and offers opportunities for realizing the special preparation of GDY according to the desired structure and unique properties. These structural characteristics and excellent physical and chemical properties of GDY have attracted increasing attention in the field of electrocatalysis. Herein, the research progress in the synthesis of atomic-level functionalized GDYs and their electrocatalytic applications are summarized. Special attention was paid to the research progress of metal-atom-anchored and nonmetallic-atom-doped GDYs for applications in the oxygen reduction reaction (ORR), the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) catalytic processes. In addition, several potential development prospects and challenges of these 2D highly conjugated electron-rich full-carbon materials in the field of electrocatalysis are presented.

Nitrogen‐Rich Carbonaceous Materials for Advanced Oxygen Electrocatalysis: Synthesis, Characterization, and Activity of Nitrogen Sites

“…[287,288] Particularly, N-doped GDY has been widely investigated for electrochemical applications, including ORR electrocatalysis. [289] In 2018, Zhao et al introduced sp-hybridized nitrogen (sp-N) atoms into the skeleton of 2D GDY by a pericyclic reaction route to facilitate O 2 adsorption as well as electron transfer. [290] Corresponding TEM and polarization curves in the ORR potential region are displayed in Figure 16a-c.…”

Application of 1D/2D carbon material supported metal nanoclusters for electrochemical conversion

“…76 Next, the strong interaction between the metal and GDY results in a uniform distribution of the metal and prevents aggregation, which contributes to the long-term stability of the electrocatalytic reaction. 77–79 Finally, the presence of two acetylene bonds in GDY leads to doubling of the length of the carbon chain connecting the six-membered ring, 80–82 and this large pore formed by six acetylene bonds is very favorable for the loading of metal nanoclusters. 83…”

Electroless Deposition of Palladium Nanoparticles on Graphdiyne Boosts Electrochemiluminescence

“…Graphdiyne (GDY), a novel two-dimensional carbon allotrope, contains sp 2 and sp hybridized carbon atoms with highly π–π conjugated structure and electron transfer capability. − The unique alkyne-rich structure and π-electronic structure of GDY essentially make it a promising substrate for anchoring and stabilizing metals or metal oxides with strong d−π interactions. ,− Compared with the conventional catalyst substrates, GDY can significantly improve the catalytic efficiency and durability of catalysts used in redox reactions, electrocatalysis, photocatalysis, and water splitting catalysis. − The alkyne bond in GDY can regulate the electronic properties of loaded metal atoms, thereby improving the catalytic activity. − The strong interaction between metal atoms and GDY results in a uniform distribution and less aggregation of metal particles, leading to the long-term stability of the electrocatalytic reactions. The interfacial interaction between different components is the key factor affecting the catalytic performance, where the electronic metal–support interaction (EMSI) plays an important role in improving the catalytic activity of metal-based catalysts. − EMSI is a bridge between theoretical electronic study and heterogeneous catalyst design.…”