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Interfacial electrochemical methods focus on the phenomena occurring at the boundary between an electrode and a solution, as opposed to bulk methods that concentrate on the solution's overall properties. These interfacial methods are classified as either static or dynamic based on the presence of a nonzero current in the electrochemical cell and the consistency of analyte concentrations. Static methods, such as potentiometry, measure the cell's potential without any significant current...
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Interfacial Diffusion-Reaction Coupling Strategy for CO2 Reduction on Copper Surface in Acidic Medium.

Xinyu Chai1, Pengfei Shi2,3, Jinyu Zhao2

  • 1State Key Laboratory of Green Papermaking and Resource Recycling, School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Rd., Shanghai, 200240, China.

Angewandte Chemie (International Ed. in English)
|July 25, 2025
PubMed
Summary

Researchers developed a novel copper catalyst with a strong polarized layer for efficient carbon dioxide electroreduction reaction (CO2RR) in acidic media. This breakthrough achieves high C2+ product selectivity and stability, overcoming previous limitations in CO2 conversion.

Keywords:
Acidic mediumAzuleneDiffusion kineticsLewis basePolarization

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Traditional CO2 electroreduction (CO2RR) in neutral/alkaline solutions faces low efficiency due to bicarbonate accumulation.
  • CO2RR in acidic media offers an alternative but still requires improved conversion efficiency.
  • Developing efficient catalysts for CO2RR in acid is crucial for sustainable chemical production.

Purpose of the Study:

  • To develop a novel electrode for CO2RR in acidic media with enhanced efficiency and selectivity.
  • To investigate the mechanism by which a strong polarized layer influences CO2 diffusion and reaction kinetics.
  • To establish a new strategy for improving CO2RR performance by interfacial engineering.

Main Methods:

  • Fabrication of a copper (Cu) electrode modified with a sp3-hybridized nitrogen (sp3-N)-enriched azulene-based polymer.
  • Electrochemical characterization of the modified electrode for CO2RR in acidic medium.
  • In situ spectroscopic studies to probe the reaction intermediate and micro-environment.
  • Density Functional Theory (DFT) calculations to elucidate the reaction mechanism and energy barriers.

Main Results:

  • The modified Cu electrode achieved a high C2 Faradaic efficiency of nearly 84% at 200 mA cm-2.
  • The electrode demonstrated long-term stability, operating for over 40 hours, a record for acidic CO2RR.
  • In situ experiments revealed that the polarized layer enhances local CO2/H2O ratio and stabilizes the *CO intermediate.
  • Theoretical calculations confirmed that the polarized layer lowers the C-C coupling energy barrier.

Conclusions:

  • A strong polarized layer on Cu electrodes significantly enhances CO2RR performance in acidic media.
  • The sp3-N-enriched azulene polymer acts as a Lewis base, boosting CO2 diffusion and stabilizing key intermediates.
  • This work presents an effective interfacial diffusion-reaction coupling strategy for high-selectivity CO2RR.