In-Situ Probing CO Activation in Sulfur-Enhanced Paired Electrocatalysis for CO₂-to-C₂₊ Conversion with Alcohol...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Advanced electrocatalysts are crucial for sustainable energy solutions, enabling efficient chemical transformations.
• Simultaneous electrochemical carbon dioxide reduction (CO2RR) and alcohol oxidation (AOR) offer a pathway to valuable chemical production.

Purpose of the Study:

• To develop a practical approach for simultaneous CO2RR and AOR using a novel electrocatalyst.
• To achieve selective production of high-value chemicals with high efficiency and stability.

Main Methods:

• Fabrication of a self-supported electrocatalyst: sulfur-enhanced CuBi2O4 nanospheres on NrGO nanosheets (SCB/NG).
• Electrochemical performance evaluation for CO2RR and AOR.
• In situ Raman spectroscopy and Density Functional Theory (DFT) calculations for mechanistic insights.
• Integration into a solar-powered platform for solar-to-fuel conversion efficiency assessment.

Main Results:

• The SCB/NG electrocatalyst achieved a Faradaic efficiency for C2+ products (FEC2+) exceeding 92.4% over 200 hours.
• Demonstrated near-total selectivity for benzaldehyde and >83% selectivity for furfural.
• Mechanistic studies revealed CO dimerization and key intermediate coverage.
• The integrated solar-powered system achieved 16% solar-to-fuel conversion efficiency with >98% retention.

Conclusions:

• The developed bifunctional electrocatalyst enables efficient and selective simultaneous CO2RR and AOR.
• The study provides deep mechanistic understanding of the reaction pathway.
• The integrated solar-driven system offers a scalable strategy for CO2 utilization and high-value chemical production, advancing energy-efficient, carbon-neutral technologies.