Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

The electrocatalytic nitrogen reduction reaction (e-NRR) is a promising alternative method for the Haber-Bosch process. However, it still faces many challenges in searching for high activity, stability, and selectivity catalysts and ascertaining the catalytic mechanism with complete insight. Here, a series of graphene-based N-bridged dual-atom catalysts (M1-N-M2/NC) are systematically investigated via first-principle calculation and a high-throughput screening strategy. The result unveils that N2 adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts (SACs). Moreover, V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts, with extremely low limiting potentials of -0.20 and -0.18 V, respectively. Furthermore, the adsorption site competition between *N2 and *H, as well as the competitive twin reactions of hydrogen evolution reaction (HER) on intermediates (NnHm) during the e-NRR process, is systematically evaluated to form a remodeling insight for the reactions in mechanism, and the e-NRR of new proposed dual-atom catalysts (DACs) is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism. This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.