Revealing the adsorption mechanisms of nitroxides on ultrapure, metallicity-sorted carbon nanotubes

Georgina Ruiz-Soria, Alejandro Pérez Paz, Markus Sauer, Duncan John Mowbray, Paolo Lacovig, Matteo Dalmiglio, Silvano Lizzit, Kazuhiro Yanagi, Angel Rubio, Andrea Goldoni, Paola Ayala, Thomas Pichler

Research output: Contribution to journalArticlepeer-review

28 Citations (Scopus)

Abstract

Carbon nanotubes are a natural choice as gas sensor components given their high surface to volume ratio, electronic properties, and capability to mediate chemical reactions. However, a realistic assessment of the interaction of the tube wall and the adsorption processes during gas phase reactions has always been elusive. Making use of ultraclean single-walled carbon nanotubes, we have followed the adsorption kinetics of NO2 and found a physisorption mechanism. Additionally, the adsorption reaction directly depends on the metallic character of the samples. Franck-Condon satellites, hitherto undetected in nanotube-NOx systems, were resolved in the N 1s X-ray absorption signal, revealing a weak chemisorption, which is intrinsically related to NO dimer molecules. This has allowed us to identify that an additional signal observed in the higher binding energy region of the core level C 1s photoemission signal is due to the Cî-O species of ketene groups formed as reaction byproducts. This has been supported by density functional theory calculations. These results pave the way toward the optimization of nanotube-based sensors with tailored sensitivity and selectivity to different species at room temperature.

Original languageEnglish
Pages (from-to)1375-1383
Number of pages9
JournalACS Nano
Volume8
Issue number2
DOIs
Publication statusPublished - Feb 25 2014
Externally publishedYes

Keywords

  • X-ray absorption
  • carbon nanotube sensors
  • chemisorption
  • photoemission
  • physisorption

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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