High degree of N-functionalization in macroscopically assembled carbon nanotubes

McGlynn, Ruairi J. and Brunet, Paul and Chakrabarti, Supriya and Boies, Adam and Maguire, Paul and Mariotti, Davide (2022) High degree of N-functionalization in macroscopically assembled carbon nanotubes. Journal of Materials Science, 57. 13314–13325. ISSN 0022-2461 (https://doi.org/10.1007/s10853-022-07463-7)

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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.

ORCID iDs

McGlynn, Ruairi J., Brunet, Paul, Chakrabarti, Supriya, Boies, Adam, Maguire, Paul and Mariotti, Davide ORCID logoORCID: https://orcid.org/0000-0003-1504-4383;