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Summary

We developed a novel bismuth-based catalyst with dual-wettability nanodomains to improve carbon dioxide electroreduction. This catalyst enhances selectivity and stability for formate production at industrial rates.

Keywords:
CO2 electroreductionFormateInterfacial wettabilityMicroenvironment modulationTriple‐phase boundary

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Precise control of interfacial water structure is crucial for selective CO2 electroreduction.
  • Industrial current densities require suppression of side reactions like hydrogen and CO evolution.

Purpose of the Study:

  • To synthesize bismuth-based catalysts with engineered interfacial water structures.
  • To enhance selectivity and stability for CO2 electroreduction to formate.

Main Methods:

  • Synthesis of bismuth nanoparticles with embedded polyvinylidene fluoride (PVDF) to create superhydrophilic-superhydrophobic nanodomains.
  • Characterization using operando spectroscopy and multiscale simulations.
  • Electrochemical testing at industrial current densities.

Main Results:

  • The optimized Bi-PVDF catalyst demonstrated significantly enhanced formate partial current density and Faradaic efficiency (FE).
  • Achieved >90% FE at -200 mA cm-2 for 50 hours and maintained high selectivity up to -700 mA cm-2.
  • Operando spectroscopy and simulations revealed modulated local hydration and charge distribution.

Conclusions:

  • The dual-wettability interface effectively stabilizes *OCHO intermediates while suppressing side reactions.
  • This strategy addresses coupled gas-proton transport challenges for high-rate CO2 electroreduction.
  • Offers a mechanism-driven and scalable approach for designing advanced electrocatalysts.