Design for non-transition metal doped nanoribbons catalysis to achieve efficient nitrogen fixation

High percentage of N2 in the air can provide abundant nitrogen source for the ammonia industry. However, nitrogen fixation process still faces great challenges due to the stable nitrogen-nitrogen triple bond. Recently, single atom electrocatalyst (SAC) has arguably become the most promising frontier in synthetic ammonia industry due to its high activity, selectivity and stability. Specially, metal-free catalysis has attracted great attention due to the low-cost and environmentally friendly feature. Herein, we investigate a series of nitrogen reduction reaction (NRR) electrocatalysts as graphene nanoribbons (GNR) embedded by 16 kinds of non-transition metal single atom catalysis (nonTMSAC) from density functional theory (DFT) computations. The stability of this system is firstly verified by AIMD simulation and formation energies. Among all candidates, Si anchored on GNR system achieves the limiting potential as low as -0.45 V and the binding energy for NNH also serves as a good descriptor for onset potential. Electronic structure reveals that such design satisfies a “acceptance-donation” interaction scenario which is also verified by crystal orbital Hamilton population (COHP) and spatial charge distribution. This work not only proposes an effective catalysis towards NRR, but also emphasizes the origin of electronic structures which can be the guidance for future NRR research.