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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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.