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

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.