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Enhancing C2+ Product Faradaic Efficiency in CO2 Reduction Using Fluorine-Stabilized Superhydrophobic Copper (δ+).

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Fluorine incorporation into copper oxide (Cu2O) nanospheres stabilizes the active copper oxidation state, significantly enhancing selectivity for C2+ products like ethylene. This novel approach improves catalyst stability and suppresses hydrogen evolution, paving the way for efficient electrochemical CO2 reduction.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Oxide-derived (OD) Cu catalysts are effective for C2+ production but suffer from metallic state reversion, reducing selectivity.
  • Stabilizing the positive oxidation state of copper is crucial for maintaining catalyst performance.

Purpose of the Study:

  • To develop a novel strategy for incorporating fluorine (F) into Cu2O nanospheres to enhance catalyst stability and selectivity.
  • To investigate the role of fluorine in stabilizing the Cu (δ+) oxidation state and improving C2+ product formation.

Main Methods:

  • Hydrofluoric acid (HF) treatment for F incorporation into Cu2O nanospheres.
  • Characterization using 19F magic-angle spinning (MAS) solid-state nuclear magnetic resonance (ssNMR) spectroscopy, water contact angle (WCA) measurements, in situ Raman, and in situ ATR-FTIR spectroscopy.
  • Density functional theory (DFT) calculations and Bader charge analysis for mechanistic insights.

Main Results:

  • Fluorine incorporation stabilized the Cu (δ+) oxidation state, achieving 91.9 ± 2.03% Faradaic efficiency for C2+ products (67% ethylene) at 250 mA cm-2.
  • F substitution at oxygen vacancies and formation of a surface HF layer were confirmed by ssNMR.
  • Enhanced hydrophobicity (WCA = 161°) suppressed hydrogen evolution reaction (HER).
  • In situ studies confirmed prolonged Cu2O stability and elucidated the ethylene production pathway.

Conclusions:

  • Fluorine incorporation into Cu2O nanospheres is a viable strategy to stabilize the active oxidation state and enhance selectivity for C2+ products in electrochemical CO2 reduction.
  • The enhanced hydrophobicity and electronic effects of fluorine contribute to improved catalyst performance and stability.
  • This work provides a new avenue for designing advanced electrocatalysts for efficient CO2 conversion.