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

There has been an increasing interest in converting nitrogen (N-2) 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.

Automated summary

This study investigates the NRR catalytic performance of single transition metal atoms anchored on two dimensional VSe2, with W-VSe2 showing the best performance. The results suggest that the limiting potential of NRR on TM-VSe2 is negatively correlated with the adsorption energy of reaction intermediate *N-NH and related with the total magnetic moment of TM-VSe2.