First-principles study of transition metal atom doped MoS2 as single-atom electrocatalysts for nitrogen fixation

Abstract

NH₃, as a carbon-free energy carrier that can replace H₂, is also an important raw material for fertilizer. Compared with Haber–Bosch process, electrocatalytic NH₃ synthesis has the green advantage of using renewable resources under ambient conditions. Herein, the catalytic performance of 3d transition metal single atom anchored in MoS₂ (TM@MoS₂) as electrocatalyst for nitrogen reduction reaction (NRR) has been investigated by first-principles calculation. By evaluating the stability, activity and selectivity of the catalysts, V@MoS₂ was found to be a potential catalyst. After simulating the entire NRR pathway, it was found that the limiting potential was only −0.311 V, indicating that V@MoS₂ had high catalytic activity. Finally, the partial density of states, charge density difference and crystal orbital Hamilton population were calculated to reveal the reason for the high catalytic activity of V@MoS₂. We hope that this work can provide new design concepts for the development of efficient MoS₂-based electrocatalysts.