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Revealing Nafion-Induced Copper Modifications by Combining In Situ and Ex Situ X-Ray Absorption Spectroscopy.

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Nafion binder alters copper catalysts in electrochemical CO2 reduction, forming Cu2+ species and influencing product selectivity. In situ X-ray absorption spectroscopy reveals these crucial catalyst-binder interactions.

Keywords:
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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Electrochemical CO2 reduction (CO2RR) using Cu-based catalysts is key for producing multi-carbon products.
  • Nafion is a common proton-conductive binder in CO2RR catalysts, ensuring mechanical stability.

Purpose of the Study:

  • To investigate the impact of Nafion on the initial oxidation state of Cu catalysts during CO2RR.
  • To elucidate catalyst-binder interactions using in situ characterization.

Main Methods:

  • In situ soft X-ray absorption spectroscopy (XAS) to probe catalyst dynamics.
  • Ex situ Cu K-edge measurements for corroboration.
  • Faradaic efficiency measurements to assess product selectivity.

Main Results:

  • Nafion alters the Cu catalyst's chemical environment, forming Cu2+ species likely due to ionomer acidity and coordination with sulfonic groups.
  • Spin-coating Nafion enhances CO and ethylene production compared to drop-casting.
  • Both methods favor HCOOH as the primary product.

Conclusions:

  • Nafion acts as both a structural binder and an active modifier of catalytic behavior.
  • In situ XAS is vital for understanding catalyst-binder interactions in CO2RR.
  • The method of Nafion application significantly impacts CO2RR product selectivity.