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Here, we report the direct cyanation of aromatic substrates using N\n                    <jats:sub>2<\/jats:sub>\n                    and methane (CH\n                    <jats:sub>4<\/jats:sub>\n                    ) at atmospheric pressure facilitated by a custom-built, air-free dielectric barrier discharge (DBD) plasma system. A broad range of aromatic compounds, including benzene, were successfully transformed into their corresponding aromatic nitriles. Both experimental and computational evidence suggested that the reaction proceeds primarily via the in situ generation of \u2022CN radicals from N\n                    <jats:sub>2<\/jats:sub>\n                    and CH\n                    <jats:sub>4<\/jats:sub>\n                    within the plasma zone. Subsequent radical addition to aromatic rings allowed the one-pot formation of aryl nitriles. This approach represents a major advancement in dinitrogen-based organic methodologies, providing an efficient alternative to conventional cyanation methods that heavily rely on lengthy synthetic routes and hazardous cyanide reagents.\n                  <\/jats:p>","DOI":"10.1126\/sciadv.ady3414","type":"journal-article","created":{"date-parts":[[2026,2,20]],"date-time":"2026-02-20T18:58:58Z","timestamp":1771613938000},"update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":1,"title":["Direct cyanation of aromatic rings using dinitrogen and methane promoted by nonthermal plasma"],"prefix":"10.1126","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-7721-3934","authenticated-orcid":true,"given":"Lei","family":"Yu","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences (BNLMS), Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, College of 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