Fe, V-co-doped C2N for electrocatalytic N2-to-NH3 conversion

Designing providential catalyst is the key to drive the electrochemical nitrogen reduction reactions (NRR), which is referring to multiple intermediates and products. By means of density functional theory (DFT) calculations, we studied heteronuclear bi-atom electrocatalyst (HBEC) for NRR. Our results revealed that compared to homonuclear bi-atom electrocatalyst (Fe2@C2N, V2@C2N), Fe, V-co-doped C2N ([email protected]2N) had a smaller limiting potential of −0.17 V and could accelerate N2-to-NH3 conversion through the enzymatic pathway of NRR. Importantly, NN bond length monotonically increases with increasing the Bader charges of adsorbed N2 molecule but decreases with increasing the Bader charge difference of two adsorbed N atoms. Additionally, the [email protected]2N could suppress the production of H2 by the preferential adsorption and reduction of N2 molecule. Thus, the as-designed HBEC may have the outstanding electrochemical NRR performance. This work opens a new perspective for NRR by HBECs under mild conditions.