Phosphorus-Doped Cu/Fe₂O₃ Electrocatalysts with Optimized Synergy between the Different Sites for Efficient Urea...

Area of Science:

• Electrochemistry
• Materials Science
• Sustainable Chemistry

Background:

• Urea electrosynthesis from CO2 and NO3- (UECN) presents a sustainable alternative to conventional methods.
• Designing electrocatalysts for high Faradaic efficiency (FE) and urea yield rates in UECN remains a challenge.

Purpose of the Study:

• To develop an advanced electrocatalyst for efficient urea electrosynthesis.
• To investigate the mechanism behind enhanced UECN performance.

Main Methods:

• Synthesis of a phosphorus-doped Cu/Fe2O3 electrocatalyst (P-Cu/Fe2O3).
• Electrochemical performance testing of UECN.
• Operando spectroscopic characterization and density functional theory (DFT) simulations.

Main Results:

• P-Cu/Fe2O3 achieved a high FE of 73.81% and a urea yield rate of 62.74 mmol h-1 g-1cat. at -0.68 V vs RHE.
• Urea yield rate increased to 97.11 mmol h-1 g-1cat. at -0.88 V vs RHE.
• DFT simulations revealed P doping modulates electronic structure, promoting key intermediate formation and hydrogenation.

Conclusions:

• The P-Cu/Fe2O3 electrocatalyst demonstrates superior UECN performance.
• P doping facilitates a multisite cooperative mechanism for enhanced urea synthesis.
• This work offers a new strategy for designing high-performance electrocatalysts for industrial urea production.