Two-Dimensional Dirac Nodal Line Carbon Nitride to Anchor Single-Atom Catalyst for Oxygen Reduction Reaction

Two-dimensional carbon nitride (2DCN) materials have emerged as an important class of 2D materials beyond graphene. However, 2DCN materials with nodal-line semimetal characteristic are rarely reported. In this work, a new nodal-line semimetal 2DCN with the stoichiometry C₄ N₄ is designed by using density functional theory (DFT) calculations and its application to anchor single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) is investigated. C₄ N₄ is a planar covalent network (sp² hybridization) with regular holes formed by the four N atoms, which is dynamically, thermodynamically, and mechanically stable. The nodal line is contributed by the p_z orbitals of C and p_x/y orbitals of N atoms. C₄ N₄ shows an anisotropic Fermi velocity and high electron mobility. Because of its porous structure, C₄ N₄ can anchor heteroatoms as SACs for electrocatalysis. C₄ N₄ anchored with Fe or Co is shown to be highly active for the ORR with a rather high half-wave potential of around 0.90 V, which is higher than those of SACs on other carbon nitrides. These findings may provide a new strategy to design novel substrates for SACs.