High Catalyst Performance of 2D π–d Conjugated TM3B3N3S6 for Hydrogen Evolution Reaction

Single-atom catalysts (SACs) for the hydrogen evolution reaction (HER) is an efficient electrochemical pathway to produce the green production. However, the development of HER process is hampered by the lack of high-performance electrocatalysts. In this work, we proposed a new π-d conjugated structure of the Ti₃B₃N₃S₆ monolayer as the single-atom catalysts for the HER process by using the density functional theory (DFT) calculations. The calculated results show that the Ti atom is active site of the Ti₃B₃N₃S₆ monolayer with the high catalytic activity (ΔG_H = –0.14 eV) for HER. The electronic properties of the Ti₃B₃N₃S₆ monolayer were explored by the electron localization function (ELF), Bader charge analysis and the polarized density of states (PDOS) density analysis. The Ti₃B₃N₃S₆ monolayer can promote the electronic transfer during the HER process, which indicates taht the Ti₃B₃N₃S₆ monolayer can is considered to investigate the catalytic activity for HER. The Gibbs free energy of H atoms adsorption on the Ti₃B₃N₃S₆ monolayer is –0.14 eV. Furthermore, the origin of high catalytic activity for the Ti₃B₃N₃S₆ monolayer was explored by the analysis the PDOS of the H adsorption on the Ti₃B₃N₃S₆ monolayer. Therefore, our work propose a new and high catalytic single-atom catalyst for the HER.