Phosphorus-Mediated Oxygen Vacancy Engineering in Cu₂O for Highly Selective CO₂ Electroreduction to Multicarbon...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Copper (Cu)-based electrocatalysts are crucial for CO2 electroreduction to multicarbon (C2+) products.
• High C2+ selectivity at industrial current densities remains a challenge for Cu-based catalysts.

Purpose of the Study:

• To develop a phosphorus (P)-doping strategy to enhance CO2 electroreduction performance in Cu2O.
• To investigate the mechanism by which P-doping improves C2+ selectivity and current density.

Main Methods:

• Phosphorus doping of Cu2O electrocatalysts.
• Electrochemical performance testing at high current densities.
• In situ Raman spectroscopy and density functional theory (DFT) calculations for mechanistic studies.

Main Results:

• Achieved 87.0% C2+ Faradaic efficiency at 347.8 mA·cm-2 using P-doped Cu2O.
• P-doping dynamically creates high-density oxygen vacancies (OVs) in the Cu2O lattice.
• Optimized surface coverage of *CO intermediates and promoted C-C coupling via OV-rich structure.

Conclusions:

• P-doping mediation is an effective strategy for designing high-performance CO2 electroreduction catalysts.
• Oxygen vacancies play a critical role in enhancing both activity and selectivity for C2+ products.
• This work offers atomic-level insights into defect engineering for advanced CO2 conversion systems.