Synergistic ultra-high activity of double B doped graphyne for electrocatalytic nitrogen reduction

The electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is an emerging technique to address energy shortages and climate change. Thus, developing efficient but low-cost electrocatalysts is important. In the present paper, we applied gamma-graphyne (gamma Gy) doped with B, N, O, P and S as NRR catalysts, and the activities of these catalysts were studied by extensive density functional theory (DFT) calculations. Our results suggest that single N, O, P and S doping are not effective in enhancing gamma Gy NRR activity, and the gamma Gy with B (sp(2))-C(sp)-B(sp) configuration has excellent overall NRR activity with a record low limiting potential (-0.12 V), good conductivity, low hydrogen evolution reaction activity and high dynamic stability. We revealed that the spC directly connected to active sp-B can be an energy buffer that makes a flat potential energy surface. Overall, our research provides several good NRR catalysts by carefully controlling the doping sites and provides a new strategy for further development of metal-free catalysts for the NRR.

Automated summary

This study focuses on developing efficient and low-cost electrocatalysts for the nitrogen reduction reaction (NRR) under ambient conditions. By doping gamma-graphyne with B, N, O, P, and S, the researchers identified a specific configuration that exhibited excellent NRR activity. The findings provide insight into improving NRR activity and offer a new strategy for developing metal-free catalysts for this reaction.