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•The nitrogen reduction reaction (NRR) on the newly-reported 2D-Fe2C12 materials is probed.•The coupling cooperation of closely arranged Fe atoms gives higher spin moment and d band center.•2D-Fe2C12 monolayer with the atomically dispersed Fe atoms in the same side possesses high activity and selectivity toward N2 reduction to NH3.
Development of high-performance and eco-friendly electrocatalysts for N2 reduction to NH3 is receiving considerable attention. Here the nitrogen reduction reaction (NRR) on the newly-reported 2D-Fe2C12 materials has been intensively investigated using density functional theory (DFT). We found that the 2D-Fe2C12 monolayer with atomically dispersed Fe atoms on the same side, denoted as 1s-Fe2C12, possessing high activity and selectivity toward NRR due to the cooperative interaction of two adjacent individual Fe active sites. The NRR channel starting from the bridge-on adsorbed configuration *N-*N has a low onset potential of −0.58 V, and this value could be further reduced to −0.40 V by including the solvation effect. The relatively large energy differences of ∼−0.3 eV for ΔG(*N2)-ΔG(*H) and the almost neutral value for ΔG(*H)-ΔG(*N2→*N-*NH) guarantee the high selectivity for NRR on 1s-Fe2C12. These findings suggest that 1s-Fe2C12 should have great potential for the design of highly efficient electrocatalysts for NRR.