Characterization of Complex Interactions at the Gas-Solid Interface with in Situ Spectroscopy: The Case of Nitrogen-Functionalized Carbon

Sarah Shulda, Thomas Gennett, Michael Dzara, Kateryna Artyushkova, Matthew Strand, Chilan Ngo, Ethan Crumlin, Svitlana Pylypenko

Research output: Contribution to journalArticlepeer-review

17 Scopus Citations

Abstract

Interactions at the gas-solid interface drive physicochemical processes in many energy and environmental applications; however, the challenges associated with characterization and development of these dynamic interactions in complex systems limit progress in developing effective materials. Therefore, structure-property-performance correlations greatly depend on the development of advanced techniques and analysis methods for the investigation of gas-solid interactions. In this work, adsorption behavior of O2 and humidified O2 on nitrogen-functionalized carbon (N-C) materials was investigated to provide a better understanding of the role of nitrogen species in the oxygen reduction reaction (ORR). N-C materials were produced by solvothermal synthesis and N-ion implantation, resulting in a set of materials with varied nitrogen amount and speciation in carbon matrices with different morphologies. Adsorption behavior of the N-C samples was characterized by in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and ambient pressure X-ray photoelectron spectroscopy (AP-XPS) experiments. A new analysis method for the interpretation of AP-XPS data was developed, allowing both the determination of overall adsorption behavior of each N-C material and identification of which nitrogen species were responsible for adsorption. The complementary information provided by in situ DRIFTS and AP-XPS indicates that O2 adsorption primarily takes place on either electron-rich nitrogen species like pyridine, hydrogenated nitrogen species, or graphitic nitrogen. Adsorption of O2 and H2O occurs competitively on solvothermally prepared N-Cs, whereas adsorption of H2O and O2 occurs at different sites on N-ion implanted N-Cs, highlighting the importance of tuning the composition of N-C materials to promote the most efficient ORR pathway.

Original languageAmerican English
Pages (from-to)9074-9086
Number of pages13
JournalJournal of Physical Chemistry C
Volume123
Issue number14
DOIs
StatePublished - 11 Apr 2019

Bibliographical note

Publisher Copyright:
© 2019 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-73888

Keywords

  • carbon
  • digital storage
  • electrolytic reduction
  • fourier transform infrared spectroscopy
  • ion implantation
  • nitrogen
  • phase interfaces
  • spectrum analysis
  • x-ray photoelectron spectroscopy

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