Single-Step Synthesis of Fe-Fe3 O4 Catalyst for Highly Efficient and Selective Electrochemical Nitrogen Reduction

Abstract

Nitrogen reduction electrocatalysts are highly attractive for catalytic science. However, most electrocatalysts are limited by their low faradaic efficiency, poor ammonia yield, and tedious and costly catalyst synthesis process. In this work, Fe-based oxide composite nanoparticles with steady chemical states are prepared by a single-step green procedure under ambient conditions. The resulting Fe-Fe₃ O₄ demonstrates remarkable activity and selectivity for nitrogen reduction reaction (NRR) with the highest faradaic efficiency of 53.2±1.8 % and NH₃ yield rate of 24.6±0.8 μg h^-1 mg_cat. ^-1 at -0.4 V (vs. RHE) in 0.1 m Na₂ SO₄ electrolyte. Characterization experiments and theoretical calculation reveal that Fe-Fe₃ O₄ exhibits significantly enhanced charge transfer capability and suppresses the competitive HER process.

Keywords: ammonia; density functional calculations; electrocatalysis; iron; nitrogen reduction.