Three-Phase Electrolysis by Gold Nanoparticle on Hydrophobic Interface for Enhanced Electrochemical Nitrogen Reduction Reaction.

Electrochemical nitrogen reduction reaction (NRR) provides a facile and sustainable strategy to produce ammonia (NH) at ambient conditions. However, the low NH yield and Faradaic efficiency (FE) are still the main challenges due to the competitive hydrogen evolution reaction (HER). Herein, a three-phase electrocatalyst through in situ fabrication of Au nanoparticles (NPs) located on hydrophobic carbon fiber paper (Au/o-CFP) is designed. The hydrophobic CFP surface facilitates efficient three-phase contact points (TPCPs) for N (gas), electrolyte (liquid), and Au NPs (solid). Thus, concentrated N molecules can contact the electrocatalyst surface directly, inhibiting the HER since the lowered proton concentration and overall enhancing NRR. The three-phase Au/o-CFP electrocatalyst presents an excellent NRR performance with high NH yield rate of 40.6 µg h mg at -0.30 V and great FE of 31.3% at -0.10 V versus RHE (0.1 m NaSO). The N-bubble contact angle result and cyclic voltammetry analysis confirm that the hydrophobic interface has a relatively strong interaction with N bubble for enhanced NRR and weak electrocatalytic activity for HER. Significantly, the three-phase Au/o-CFP exhibits excellent stability with a negligible fluctuation of NH yield and FE in seven-cycle test. This work provides a new strategy for improving NRR and simultaneously inhibiting HER.