The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N_2 reduction reaction

摘要

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 (TM@GDY) has been systematically investigated as nitrogen (N-2) Reduction Reaction (NRR) by Density Functional Theory (DFT). The results reveal that Mo-embedded graphdiyne monolayer (Mo@GDY) 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, Mo@GDY can also effectively suppress the Hydrogen Evolution Reaction (HER) during the entire NRR process. This study may provide a new approach for electrochemical N-2 reduction to form NH3 at ambient conditions.