Efficient electrocatalytic H₂ evolution mediated by 2D Janus MoSSe transition metal dichalcogenide

Recently, 2D JTMDs with asymmetric electronic structures are inviting an intense research interest in modern science and technology. Using the first principles-based periodic hybrid dispersion-corrected Density Functional Theory (DFT-D) method, we have investigated equilibrium structure, geometry, properties of monolayer MoSSe JTMD electrocatalytic activities for H2 evolution reaction (HER). We performed non-periodic quantum mechanical DFT computations to find out most favorable HER pathway on exposed surfaces Janus material i.e., Mo-edges S- or Se-edges. To explore mechanism, pathways barriers, considered a cluster model system Mo10S12Se9 illustrate Se-edges material. The present study reveals that Volmer-Heyrovsky mechanism is thermodynamically evolute at Se-terminated Mo-edges. It was found change free energy barrier during Heyrovsky about 3.93-7.10 kcal.mol-1 (in both gas solvent phases), indicating exceptional electrocatalyst lowest activation barriers. This showed Tafel slope (m) lower case due overlap s-orbital hydrogen d-orbitals Mo atoms appeared HOMO LUMO transition state TS1 H-migration step. better stabilization atomic orbitals rate-limiting step phase) key reducing barrier, thus overall catalysis performance evolution.