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 the traditional Haber−Bosch process, which consumes a lot of energy and causes serious pollution to the environment, electrocatalytic NH3 synthesis has the green advantage of using renewable resources to react under ambient conditions. In this study, the catalytic performance of 3d transition metal single atom anchored in MoS2 (TM@MoS2) as electrocatalyst for nitrogen reduction reaction (NRR) has been systematically 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, crystal orbital Hamilton population, and Bader charge transfer were calculated to reveal the reason for the high catalytic activity of V@MoS2. We hope that this work will provide new design concepts for the development of efficient MoS2-based electrocatalysts for the NRR.

Keywords: Nitrogen reduction reaction, Electrocatalysts, MoS2, DFT calculations, Dope