High degree of N-functionalization in macroscopically assembled carbon nanotubes

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Abstract: Nitrogen doping of carbon nanomaterials has emerged as a method to develop novel material properties, though limitations in the form of extended treatment times, harsh chemical usage and limited total nitrogen content exist. Here, macroscopic ribbon-like assemblies of carbon nanotubes are functionalized with nitrogen using a simple direct current-based plasma–liquid system. This system utilizes the plasma-generated species in an ethanol:water solution with ethylenediamine as a nitrogen precursor for the nitrogen functionalization of the carbon nanotube assembly. These unique, plasma-generated species and pathways enable rapid and high levels of functionalization with the atomic concentration of nitrogen reaching 22.5%, with amine groups, pyrrolic groups and graphitic nitrogen observed in the X-ray photoelectron spectra, the highest ever achieved. This nitrogen content is demonstrated to be significantly higher than a comparative electrolysis process. This demonstrates that this plasma process enhances the availability of nitrogen from the ethylenediamine precursor, facilitating greater functionalization. Graphical abstract:
Original languageEnglish
Pages (from-to)13314-13325
Number of pages12
JournalJournal of Materials Science
Issue number28
Early online date15 Jul 2022
Publication statusPublished - 31 Jul 2022


  • Chemical Routes to Materials
  • Chemical routes to materials


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