Ordered Mesoporous C₃N₅ with a Combined Triazole and Triazine Framework and Its Graphene Hybrids for the Oxygen Reduction Reaction (ORR)

Mesoporous carbon nitrides (MCN) with C₃ N₄ stoichiometry could find applications in fields ranging from catalysis, sensing, and adsorption-separation to biotechnology. The extension of the synthesis of MCN with different nitrogen contents and chemical structures promises access to a wider range of applications. Herein we prepare mesoporous C₃ N₅ with a combined triazole and triazine framework via a simple self-assembly of 5-amino-1H-tetrazole (5-ATTZ). We are able to hybridize these nanostructures with graphene by using graphene-mesoporous-silica hybrids as a template to tune the electronic properties. DFT calculations and spectroscopic analyses clearly demonstrate that the C₃ N₅ consists of 1 triazole and 2 triazine moieties. The triazole-based mesoporous C₃ N₅ and its graphene hybrids are found to be highly active for oxygen reduction reaction (ORR) with a higher diffusion-limiting current density and a decreased overpotential than those of bulk g-C₃ N₄ .