Atomically dispersed cerium on copper tailors interfacial water structure for efficient CO-to-acetate...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrosynthesis of acetate from carbon monoxide (CO) is a promising route for renewable carbon products.
• The competing hydrogen evolution reaction (HER) limits selectivity in CO electrosynthesis.
• Developing efficient and selective catalysts is crucial for sustainable acetate production.

Purpose of the Study:

• To design and synthesize a novel catalyst for highly selective acetate electrosynthesis from CO.
• To investigate the catalytic mechanism and understand the role of cerium single atoms (Ce-SAs) in enhancing selectivity.
• To evaluate the catalyst performance under practical operating conditions.

Main Methods:

• Synthesis of a crystalline-amorphous dual-phase copper (Cu) catalyst modified with Ce-SAs.
• Electrochemical characterization including cyclic voltammetry and chronoamperometry.
• Operando spectroscopy to study reaction intermediates and surface species.
• Fabrication and testing of a flow-cell reactor for long-term stability assessment.

Main Results:

• The Ce-SAs modified Cu catalyst significantly suppressed HER and promoted acetate formation.
• Ce-SAs reduced interfacial K+ ion hydrated water and H* coverage, favoring CO coupling.
• A high Faradaic efficiency of 71.3% for acetate and a current density of 110.6 mA cm⁻² were achieved.
• The catalyst demonstrated stable acetate production for over 138 hours in a flow cell with >60% selectivity.

Conclusions:

• The Ce-SAs modified dual-phase Cu catalyst offers a highly selective and efficient pathway for acetate electrosynthesis from CO.
• The catalyst design strategy effectively manipulates surface properties to enhance target product formation.
• This work provides a promising catalyst for the sustainable production of acetate using renewable electricity.