Fe, V-co-doped C2N for electrocatalytic N-2-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 (Fe-2@C2N, V-2@C2N), Fe, V-co-doped C2N (FeV@C2N) had a smaller limiting potential of -0.17 V and could accelerate N-2-to-NH3 conversion through the enzymatic pathway of NRR. Importantly, N-N bond length monotonically increases with increasing the Bader charges of adsorbed N-2 molecule but decreases with increasing the Bader charge difference of two adsorbed N atoms. Additionally, the FeV@C2N could suppress the production of H-2 by the preferential adsorption and reduction of N-2 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. (C) 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

Automated summary

The design of providential catalyst is crucial for driving electrochemical nitrogen reduction reactions, with the potential to achieve efficient conversion of N2 to NH3. Understanding the relationship between Bader charges and N-N bond length variations can help optimize catalyst design.