Two-dimensional graphitic metal carbides: structure, stability and electronic properties

Abstract

Abstract Via first-principles computational modeling and calculations, we propose a new class of two-dimensional (2D) atomically thin crystals that contain metal-C3 (MC3) moieties periodically distributed in a graphenic lattice, which we refer to as 2D graphitic metal carbides (g-MCs). Most g-MCs are dynamically stable as verified by the calculated phonon spectra. Our detailed chemical bonding analyzes reveal that the high stability of g-MCs can be attributed to a unique bonding feature, which manifests as the carbon-backbone-mediated metal–metal interactions. These analyzes provide new insights for understanding the stability of 2D materials. It is found that the calculated electronic band gaps and magnetic moments (per unit cell) of g-MCs can range from 0 to 1.30 eV and 0 to 4.40 μ B, respectively. Highly tunable electronic properties imply great potential of 2D g-MCs in various applications. As an example, we show that 2D g-MnC can be an excellent electrocatalyst towards CO2 reductive reaction for the formation of formic acid with an exceptionally high loading of Mn atoms (∼43 wt%). We expect this work to simulate new experiments for fabrication and applications of g-MCs.