High-density Fe single atoms anchored on 2D-Fe2C12 monolayer materials for N2 reduction to NH3 with high activity and selectivity

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 selec-tivity 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 triangle G(*N-2)-triangle G(*H) and the almost neutral value for triangle G(*H)-triangle G(*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.

Automated summary

This study investigates the nitrogen reduction reaction (NRR) on 2D-Fe2C12 materials and finds that the 1s-Fe2C12 monolayer exhibits high activity and selectivity due to the cooperative interaction of adjacent Fe active sites. The results suggest that 1s-Fe2C12 has great potential for designing efficient electrocatalysts for NRR.