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.