Revealing the importance of nitrogen doping site in enhancing the oxygen reduction reaction on β-graphyne

In the present paper, density functional theory calculations were carried out on a detailed oxygen reduction reaction (ORR) process catalysed by nitrogen-doped β-graphyne (βGy). Nitrogen-doping can increase the positive charge of the adjacent carbon atom and the graphyne work function, promoting O₂ decomposition. Our calculations revealed that N-doped βGy can efficiently facilitate the ORR process via a four-electron mechanism, regardless of doping position. Additionally, our results revealed that the N doping site was essential for tuning the ORR catalytic activity. N1 doping was shown to more effectively promote the ORR than N2 doping. In addition, our research enhances the current understanding of catalytic activity at the molecular level.