The FeN 3 Doped Fluorographene for N 2 Fixation: A Density Functional Theory Study

The ammonia synthesis under ambient condition is of significance for sustainable energy utilization. Herein, the nitrogen reduction reaction (NRR) on FeN 3 embedded graphane and fluorographene are investigated by density functional theory calculations. Our results indicate that the functional fluorographene accelerates electrocatalytic N 2 fixation with an onset‐potential of 0.97 V via alternating mechanism, being superior to the graphane counterpart. Furthermore, the fluorination alleviates the H poisoning and increases NRR selectivity. The improved performance is originated from the strong electron‐withdrawing of the F decoration. Moreover, the inferior NRR performance of the FeN 3 decorated graphane indicates the infeasibility as the NRR electrode, reasonably avoiding the experimental attempt. This finding opens up the new design for the carbon‐based electrocatalysts with high efficiency of NH 3 synthesis.