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N\u2010CNT catalyze the reductive N\u2010methylation of nitro\u2010 and dinitrobenzenes and nitrotoluenes to the corresponding N\u2010methyl and N,N\u2010dimethyl amines when methanol is used as the solvent. N\u2010CNT were synthesized via a chemical vapor deposition method using acetonitrile over a Ni\/CaO catalyst. The obtained N\u2010CNT were characterized by transmission electron microscopy, scanning electron microscopy, x\u2010ray diffraction, Raman spectroscopy, x\u2010ray photoelectron spectroscopy, nitrogen adsorption\/desorption, thermogravimetric analysis, and Fourier\u2010transform infrared spectroscopy. The influence of surface carboxyl functional groups and nitrogen doping of carbon nanotubes on hydrogenation and N\u2010methylation reactions is demonstrated. The results provide the first evidence that carbon material, particularly N\u2010CNT can serve as efficient metal\u2010free catalyst for the one\u2010step synthesis of secondary and tertiary aromatic amines from the corresponding nitro compounds. The demonstrated bifunctional behavior of N\u2010CNT, which combines redox activity for nitro group reduction and acid\u2010base functionality for N\u2010alkylation, highlights their potential as sustainable alternatives to conventional metal\u2010based catalysts.<\/jats:p>","DOI":"10.1002\/asia.70750","type":"journal-article","created":{"date-parts":[[2026,4,22]],"date-time":"2026-04-22T03:41:07Z","timestamp":1776829267000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Reductive N\u2010methylation of Aromatic Nitro Compounds on N\u2013CNT"],"prefix":"10.1002","volume":"21","author":[{"given":"Vladyslav","family":"Stets","sequence":"first","affiliation":[{"name":"L. V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Sciences of Ukraine  Kyiv Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4164-3024","authenticated-orcid":false,"given":"Igor","family":"Bychko","sequence":"additional","affiliation":[{"name":"L. V. Pisarzhevskii Institute of Physical Chemistry of National Academy of Sciences of Ukraine  Kyiv Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Svitlana","family":"Sotnik","sequence":"additional","affiliation":[{"name":"Enamine Ltd.  Kyiv Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0280-8719","authenticated-orcid":false,"given":"Peter","family":"Strizhak","sequence":"additional","affiliation":[{"name":"L. V. 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