Lithium Vacancy-Tuned [CuO₄ ] Sites for Selective CO₂ Electroreduction to C₂₊ Products

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Electrochemical CO2 reduction to C2+ products is challenging due to inefficient C-C coupling.
• Developing selective and active catalysts is crucial for sustainable chemical synthesis.

Purpose of the Study:

• To develop a lithium vacancy-tuned Li2CuO2 catalyst for enhanced electrochemical CO2 reduction.
• To investigate the effect of lithium vacancies on C-C coupling and catalytic performance.

Main Methods:

• Electrochemical delithiation to create lithium vacancies in Li2CuO2.
• Density functional theory (DFT) calculations to understand the mechanism.
• Electrochemical testing to evaluate catalytic activity and selectivity.

Main Results:

• Lithium vacancies in Li2CuO2 shorten interlayer distances and lower the CO-CO coupling energy barrier.
• The optimized Li2-xCuO2 catalyst achieved 90.6% Faradaic efficiency for C2+ products at -0.85 V.
• An outstanding partial current density of -706 mA cm-2 was achieved for C2+ products.

Conclusions:

• Lithium vacancy tuning is an effective strategy to enhance Cu-based catalysts for CO2 reduction.
• The developed catalyst shows high potential for selective production of multi-carbon chemicals from CO2.
• This work offers a new avenue for designing advanced catalysts for CO2 valorization.