Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles.

Area of Science:

• Electrochemistry
• Catalysis
• Materials Science

Background:

• Electrocatalytic CO2/CO reduction is a key area for producing valuable C2+ products.
• Achieving high selectivity for a single C2+ product remains a significant challenge in electrocatalysis.

Purpose of the Study:

• To develop a novel copper (Cu) atomic ensemble catalyst for selective electrocatalytic CO-to-acetate conversion.
• To investigate the structure-performance relationship of the Cu atomic ensemble in CO electroreduction.

Main Methods:

• Synthesis of a Cu atomic ensemble catalyst with specific site distance and coordination environment.
• Electrochemical testing to evaluate acetate Faradaic efficiency, partial current density, and CO conversion rate.
• Experimental and theoretical investigations to elucidate the reaction mechanism.

Main Results:

• The Cu atomic ensemble achieved an acetate Faradaic efficiency of 70.2% with a partial current density of 225 mA cm-2.
• A single-pass CO conversion rate of 91% and remarkable stability were demonstrated.
• The catalyst optimized C-C coupling, stabilized the key ketene intermediate (*CCO), and inhibited the *HOCCOH intermediate.

Conclusions:

• The Cu atomic ensemble effectively switches the CO reduction pathway towards acetate production.
• This catalyst design offers a promising strategy for selective electrocatalytic conversion of CO to valuable chemicals.