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Ian Kendrick1, Dunesh Kumari, Adam Yakaboski

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Summary
This summary is machine-generated.

Nafion functional groups on platinum surfaces in fuel cells cause complex potential shifts in adsorbed CO vibrations. This study reveals CF3 and SO3(-) groups directly adsorb onto platinum, influencing CO behavior.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Spectroscopy

Background:

  • Operating fuel cell electrodes feature complex interactions between Nafion ionomers and platinum catalyst surfaces.
  • The adsorption of carbon monoxide (CO) on platinum is crucial for fuel cell electrocatalysis, but its vibrational properties are sensitive to the electrode environment.
  • Understanding the role of Nafion functional groups in modifying CO adsorption is key to optimizing fuel cell performance.

Purpose of the Study:

  • To elucidate the specific Nafion functional groups responsible for the Stark tuning of CO adsorbed on platinum.
  • To investigate the coadsorption mechanisms of Nafion components at the platinum-Nafion interface.
  • To correlate experimental spectroscopic data with theoretical calculations for a comprehensive understanding.

Main Methods:

  • Operando infrared (IR) spectroscopy and polarization modulated IR spectroscopy (PM-IRRAS) were employed to study the Pt-Nafion interface.
  • Attenuated total reflectance IR spectroscopy was used for bulk Nafion analysis.
  • Density functional theory (DFT) calculations were performed to simulate and interpret experimental spectra.

Main Results:

  • DFT calculations and experimental spectra indicate that Nafion's CF3, CF2, and SO3(-) groups adsorb onto the platinum surface.
  • A proposed model of the Nafion-Pt interface suggests direct adsorption of CF3 and SO3(-) groups on platinum.
  • Mulliken partial charge calculations support CF3 coadsorption, with high charge density on CF3 fluorine atoms.

Conclusions:

  • Nafion functional groups, particularly CF3 and SO3(-), directly adsorb on platinum catalyst surfaces in operating fuel cells.
  • This coadsorption influences the ordering of Nafion backbone and side-chain CF2 groups.
  • The findings provide critical insights into the interfacial chemistry governing fuel cell electrocatalysis and performance.