Synthesis and Self‐Assembly of Ultrathin Holey Graphdiyne Nanosheets for Oxygen Reduction Reaction

Abstract

AbstractGraphdiyne (GDY) is a fascinating graphene‐like 2D carbon allotrope comprising sp and sp2 hybridized carbon atoms. However, GDY materials synthesized by solution‐phase methods normally come as thick and porous films or amorphous powders with severely disordered stacking modes that obstruct macroscopic applications. Here, a facile and scalable synthesis of ultrathin holey graphdiyne (HGDY) nanosheets is reported via palladium/copper co‐catalyzed homocoupling of 1,3,5‐triethynylbenzene. The resulting freestanding 2D HGDY self‐assembles into 3D foam‐like networks which can in situ anchor clusters of palladium atoms on their surfaces. The Pd/HGDY hybrids exhibit high electrocatalytic activity and stability for the oxygen reduction reaction which outperforms that of Pt/C benchmark. Based on the ultrathin graphene‐like sheets and their unique 3D interconnected macrostructures, Pd/HGDY holds great promise for practical electrochemical catalysis and energy‐related applications.