Self‐Assembled 3D Hierarchical Porous Hybrid as Platinum‐Like Bifunctional Nonprecious Metal Catalyst toward Oxygen Reduction Reaction and Hydrogen Evolution Reaction

Abstract A class of novel CoNC active nanoparticles anchored on 3D hierarchical porous graphene‐like carbon nanosheets compositions (CoNC@3D HPG) with high porosity, high specific surface area, interconnected pores, and a hierarchical pore structure are synthesized, which are perfect as electrochemical electrode scaffolds, giving rise to efficient and rapid pathways for ion and electron transport, which certainly facilitate the mass transport. This hybrid catalyst possesses outstanding oxygen reduction reaction (ORR) activity through a four‐electron transfer process. Most importantly, the ORR activity of this material is superior to Pt/C catalyst, better stability and fuel (methanol and CO) tolerance than Pt/C catalyst. Besides, the CoNC@3D HPG also exhibits outstanding electrocatalytic performance as an efficient hydrogen evolution reaction catalyst with zero onset overpotential, low overpotential at large current density, small Tafel slope, high exchange current density, and excellent durability. It is worth noting that this outstanding bifunctional catalyst is prepared by a novel resin‐based self‐assembly growth methodology at large‐scale.