MOF-derived Fe2O3/MoSe2 composites for promoted electrocatalytic nitrogen fixation

Abstract

Due to the low activity and poor selectivity of current artificial nitrogen fixation catalysts, there is an urgent need to develop efficient and environmentally friendly electrochemical ammonia synthesis (EAS) electrocatalysts. Electrochemical ammonia synthesis is considered an environmentally friendly and sustainable method for artificial nitrogen fixation. Herein, Fe₂O₃ nanoparticles assembled on MoSe₂ (Fe₂O₃/MoSe₂) were first developed and regarded as an efficient electrocatalytic nitrogen fixation catalyst with high electroactivity. The Fe₂O₃/MoSe₂ composites exhibited excellent NRR activity with an NH₃ yield of 46.25 μg h⁻¹ mg⁻¹ at −0.5 V and an FE of 9.6% at −0.6 V vs. RHE. Notably, the Fe₂O₃/MoSe₂ composites exhibited excellent stability and durability in recycling tests. According to the findings of density functional theory (DFT) calculations, it was discovered that the transmission of interfacial charges from Fe₂O₃ to MoSe₂ can considerably intensify the electrochemical nitrogen reduction reaction (NRR) activity of Fe₂O₃/MoSe₂ through facilitating the electrical conductivity of Fe₂O₃/MoSe₂ and lowering the free energy obstacle for the rate-determining *N₂ to *N₂H formation step. This work provides a promising avenue for the green synthesis of NH₃.