The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N2 reduction reaction

The production of ammonia (NH3) at ambient conditions has always faced enormous challenges in chemical industry. In this study, the potential of the electrocatalysts of transition-metal-embedded (TM = Sc, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd and Ag) graphdiyne monolayer ([email protected]) has been systematically investigated as nitrogen (N2) Reduction Reaction (NRR) by Density Functional Theory (DFT). The results reveal that Mo-embedded graphdiyne monolayer ([email protected]) has high stability, high electrical conductivity and excellent catalytic activity with ultra-low onset potential (−0.33 V) by distal mechanism. The ultra-low onset potential is attributed to much stronger interactions between hydrogen and the next nearest nitrogen atoms (H-N2) for the distal mechanism compared with the enzymatic mechanism (−1.03 V) during the first hydrogenation. Moreover, [email protected] can also effectively suppress the Hydrogen Evolution Reaction (HER) during the entire NRR process. This study may provide a new approach for electrochemical N2 reduction to form NH3 at ambient conditions.