Single transition metal atom anchored on VSe₂ as electrocatalyst for nitrogen reduction reaction

There has been an increasing interest in converting nitrogen (N₂) to ammonia (NH₃) via electrochemical nitrogen reduction reaction (NRR). In this study, the NRR catalytic performance of a series of single transition metal (TM) atoms anchored on two dimensional VSe₂ (TM-VSe₂) was studied via performing the first-principles calculations. Among the investigated single-atom catalyst of TM-VSe₂, W-VSe₂ demonstrates the best NRR catalytic performance with a limiting potential of −0.36 V and effective inhibition of the competitive hydrogen evolution reaction. Meanwhile, our calculations demonstrate that W-VSe₂ is highly stable as single-atom anchored on the surface of VSe₂ monolayer, whose improved electrical conductivity ensures the electron transform during NRR process. Moreover, we found that the limiting potential of NRR on TM-VSe₂ was negatively correlated with the adsorption energy of reaction intermediate *N-NH, and related with the total magnetic moment of TM-VSe₂. Importantly, we identified the origin of the NRR catalytic activity from electronic aspect. Our results provide a new way for measuring the NRR catalytic activity of single-atom catalysts.