The FeN3 Doped Fluorographene for N2 Fixation: A Density Functional Theory Study. Issue 30 (11th August 2020) - Yang, Lei
Abstract: The ammonia synthesis under ambient condition is of significance for sustainable energy utilization. Herein, the nitrogen reduction reaction (NRR) on FeN3 embedded graphane and fluorographene are investigated by density functional theory calculations. Our results indicate that the functional fluorographene accelerates electrocatalytic N2 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 FeN3 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 NH3 synthesis. Abstract : Table of contents: The performance of electrocatalytic ammonia synthesis is effectively altered by the graphene functionalization. Density functional theory calculations indicate that the graphene fluorination suppresses the H adsorption on FeN3 active site and boosts the selectivity of the nitrogen reduction reaction versus hydrogen evolution reaction, with respect to the graphane counterpart, which provides a clear guide for the experimental preparation.