Rational design synergistic metal-free dual-atom electrocatalyst for N2 to NH3 reaction on g-CN: A first principle study

The electrocatalytic nitrogen reduction reaction (NRR) for ammonia production is promising for N2 fixation under ambient conditions. Most of the previous studies focus on transition metal-based catalysts, while the metal-free-based ones have not gotten enough attention. We designed dual-site metal-free atoms anchored on g-CN for electrocatalytic NRR based on the density functional theory (DFT) calculation. Results indicated that the B and P atoms co-doped g-CN system exhibits excellent NRR performance with a low limiting potential of −0.18 V, superior to most metal-based catalysts. In addition, a synergistic effect induced by the hybridization of B and P atoms is proposed. Eventually, the selectivity, thermodynamical stability, and conductivity are investigated. All of these modulations make the [email protected] an excellent electrocatalyst. Our work provides a novel method for electrocatalytic NRR to ammonia and promotes the development of NRR.