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Tracking structural evolution: operando regenerative CeOx/Bi interface structure for high-performance CO2

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A novel CeOx/Bi interface structure, identified using operando measurements, significantly enhances electrocatalysis for carbon dioxide (CO2) reduction to formate. This active phase promotes efficient CO2 conversion under realistic conditions.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Designing efficient electrocatalysts for CO2 electroreduction requires understanding catalyst behavior under operating conditions.
  • Real-time structural evolution and mechanisms of precatalysts remain challenging to elucidate.

Purpose of the Study:

  • To investigate the structural evolution and identify the active phase of a CeO2/BiOCl precatalyst during CO2 electroreduction.
  • To understand the working mechanism of the catalyst at the atomic level.

Main Methods:

  • Operando structural measurements at multiscale levels.
  • Electrochemical performance testing (Faradaic efficiency, potential window).
  • Density functional theory (DFT) calculations.

Main Results:

  • The CeO2/BiOCl precatalyst transforms into a CeOx/Bi interface structure with enriched Ce3+ species.
  • The CeOx/Bi interface exhibits high formate selectivity (approaching 90% Faradaic efficiency) for 24 hours.
  • Enhanced performance was observed using D2O, suggesting a role for protonation.

Conclusions:

  • The CeOx/Bi interface is the true catalytically active phase for CO2 electroreduction to formate.
  • The interface promotes water activation and stabilizes key intermediates, facilitating efficient formate production.
  • This study provides insights into catalyst design for enhanced CO2 electroreduction.