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Dynamic Relocation of Copper Catalysts in Gas Diffusion Electrodes during CO2 Electroreduction.

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Copper electrocatalysts convert CO2 into valuable products. This study reveals Cu relocation in electrodes is pH-dependent, but flooding, not relocation, limits product selectivity at high current densities.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Developing technologies for CO2 conversion using renewable energy is crucial.
  • Copper (Cu) is a key electrocatalyst for converting CO2 into multicarbon (C2+) products.
  • Understanding Cu catalyst behavior in gas diffusion electrodes (GDEs) at high current densities is vital for industrial applications.

Purpose of the Study:

  • To investigate the correlation between Cu catalyst structure, chemical state, and C2+ selectivity in Cu-GDEs during CO2 reduction reactions (CO2RR).
  • To examine catalyst behavior at industrially relevant current densities (>200 mA/cm2).

Main Methods:

  • Utilized ex situ and in situ scanning X-ray fluorescence microscopy to observe Cu relocation.
  • Employed in situ X-ray absorption spectroscopy to identify chemical states (Cu1+).
  • Used online gas chromatography to monitor product selectivity and identify degradation mechanisms.

Main Results:

  • Significant Cu relocation within the GDE was observed after CO2RR.
  • Cu relocation occurs via a pH-dependent dissolution-redeposition mechanism, more pronounced at high pH.
  • Electrode flooding was identified as the primary cause for decreased C2+ selectivity over time, overshadowing Cu relocation effects.

Conclusions:

  • Cu relocation in GDEs is pH-dependent and occurs through dissolution-redeposition.
  • Electrode flooding is the main limitation for sustained C2+ selectivity in Cu-GDEs at high current densities.
  • Findings offer insights for designing stable and selective Cu-based GDEs for CO2 electrolyzers.