Solid Solution In Situ-Reconstructed Mg-Cu₂O/Cu Heterointerface for CO₂ Reduction to C₂₊ Alcohols in Neutral and...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical CO2 reduction is a promising route for sustainable production of C2+ alcohols.
• Conventional copper catalysts struggle with low selectivity and production rates for C2+ alcohols in neutral/acidic media due to C-C coupling energy barriers and competing C2H4 pathways.

Purpose of the Study:

• To develop a novel catalyst for enhanced selectivity and production rate of C2+ alcohols from CO2 reduction.
• To investigate the catalytic mechanism of the new material in neutral and acidic electrolytes.

Main Methods:

• In situ reconstruction of porous Mg-stabilized Cu2O/metallic Cu heterointerface from a mesoporous MgCuO solid solution.
• Electrochemical CO2 reduction experiments in neutral and acidic electrolytes.
• In situ spectroscopic and computational investigations.

Main Results:

• The Mg-Cu2O/Cu heterointerface facilitates *CO hydrogenation and asymmetric *CO-CHO coupling, suppressing energy-intensive *CO-CO dimerization.
• The heterostructure optimizes intermediate bonding, enhancing O-C and weakening Cu-O bonds, thus directing selectivity towards C2+ alcohols.
• Achieved remarkable Faradaic efficiencies of 70.4% (neutral) and 61.4% (acid) for C2+ alcohols at high current densities.

Conclusions:

• The developed Mg-stabilized Cu2O/Cu heterointerface catalyst demonstrates superior performance for CO2 to C2+ alcohols conversion.
• The findings provide a general framework for designing catalysts to steer reaction pathways in CO2 electrolysis.