Single – atom Fe/N-embedded graphdiyne as catalysts for hydrogen evolution reaction: A DFT approach

Abstract

The development of stable, efficient, and cost-effective electrocatalysts for the hydrogen evolution reaction (HER) is crucial for advancing sustainable hydrogen production, a key component in achieving clean energy goals and reducing reliance on fossil fuels. Recent theoretical and experimental studies have highlighted the promising performance of M-N-C (Metal-Nitrogen–Carbon) based carbon allotropes as HER electrocatalysts. In this study, we employed density functional theory (DFT) to investigate the HER catalytic activity of co-doped iron (Fe) and nitrogen (N) on graphdiyne (GDY), namely Fe,N-GDY materials. Our findings reveal that Fe,N-GDY exhibits remarkable stability, enhanced electrical conductivity, and a reduced energy gap compared to pristine GDY. The hydrogen adsorption sites on Fe,N-GDY were systematically analyzed, with hydrogen adsorption free energy ($\Delta G_{H^{\ast }}$) values approaching zero, specifically 0.020 eV for the H3@Fe,N3-GDY model, which is the closest to the well-established Pt(111) (−0.090 eV). This suggests that Fe,N-GDY offers superior catalytic performance for HER. Our results introduce Fe,N-GDY as a highly efficient electrocatalyst for HER, presenting a promising strategy for the design of advanced catalysts for sustainable hydrogen production.