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Altering catalyst support electronegativity controls electrochemical carbon dioxide reduction. High electronegativity dopants shift selectivity to valuable multicarbon products, enhancing catalyst performance and stability.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Catalyst-support interactions are crucial for controlling catalytic activity.
  • Rational design of catalyst supports is hindered by unclear property-activity relationships.
  • Electrochemical carbon dioxide reduction (CO2RR) is a key process for sustainable chemical production.

Purpose of the Study:

  • To investigate the influence of support electronegativity on reaction pathways in CO2RR.
  • To establish a clear property-activity relationship for catalyst support design.
  • To develop highly selective and stable catalysts for CO2RR.

Main Methods:

  • Fabrication of a model system using copper (Cu) nanoparticles on carbon supports with varying heteroatom dopants.
  • Systematic variation of dopant electronegativity to tune catalyst-support interactions.
  • Electrochemical characterization, including Faradaic efficiency (FE) measurements at controlled current densities.
  • Long-term stability testing and performance evaluation using simulated flue gas.

Main Results:

  • Support electronegativity directly influences electron density on Cu nanoparticles and CO2RR pathways.
  • High electronegativity dopants promote selectivity towards multicarbon products (C2+).
  • A composite Cu and fluorine-doped carbon catalyst achieved 82.5% C2+ FE at 400 mA cm-2 with 44-hour stability.
  • The developed catalyst demonstrated a 5.3-fold increase in C2+ FE using simulated flue gas compared to a reference Cu catalyst.

Conclusions:

  • Electronegativity is a critical parameter for tuning catalyst-support interactions in CO2RR.
  • This work provides a rational design principle for developing advanced CO2RR catalysts.
  • The developed F-doped carbon supported Cu catalyst shows significant potential for efficient and selective CO2 conversion.