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Instead, direct C\u2212N bond formation from dinitrogen (N<jats:sub>2<\/jats:sub>) is of great interest but remains a challenge. Here, by virtue of unique plasma\u2013liquid interactions, we developed an environmentally benign one\u2010pot approach to directly couple benzene and N<jats:sub>2<\/jats:sub>, two naturally abundant yet chemically inert molecules, into value\u2010added arylamines. Under the optimal conditions, an amination yield of 45\u2009% was rapidly achieved, far better than the reported benzene amination efficiency using ammonia. A tentative reaction mechanism was proposed involving the long\u2010lived N<jats:sub>2<\/jats:sub> (A<jats:sup>3<\/jats:sup><jats:inline-graphic xmlns:xlink=\"http:\/\/www.w3.org\/1999\/xlink\" xlink:href=\"graphic\/anie202203680-math-0001.png\" xlink:title=\"urn:x-wiley:14337851:media:anie202203680:anie202203680-math-0001\"\/>\n) and N<jats:sub>2<\/jats:sub><jats:sup>+<\/jats:sup> species, as evidenced by the key intermediates detected. With a deeper mechanistic understanding and by further optimizing the plasma reactor, the realization of cost\u2010effective electrical amination of benzene with N<jats:sub>2<\/jats:sub> could become reality.<\/jats:p>","DOI":"10.1002\/anie.202203680","type":"journal-article","created":{"date-parts":[[2022,3,25]],"date-time":"2022-03-25T03:19:57Z","timestamp":1648178397000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["Direct Amination of Benzene with Molecular Nitrogen Enabled by Plasma\u2010Liquid Interactions"],"prefix":"10.1002","volume":"61","author":[{"given":"Xia","family":"Xu","sequence":"first","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry and Materials Science Northwest University  Xi'an Shaanxi 710027 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuyang","family":"Zhao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry and Materials Science Northwest University  Xi'an Shaanxi 710027 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Tang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Transient Optics and Photonics Xi'an Institute of Optics and Precision Mechanics of CAS  Xi'an Shaanxi 710119 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixiang","family":"Duan","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry and Materials Science Northwest University  Xi'an Shaanxi 710027 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1261-3192","authenticated-orcid":false,"given":"Yong\u2010Hui","family":"Tian","sequence":"additional","affiliation":[{"name":"Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry and Materials Science Northwest University  Xi'an Shaanxi 710027 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2022,4,11]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1186120"},{"key":"e_1_2_7_2_1","unstructured":"\u00a0"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.906"},{"key":"e_1_2_7_4_2","doi-asserted-by":"publisher","DOI":"10.1038\/nature12435"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-019-1134-2"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1085326"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201603142"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201603142"},{"key":"e_1_2_7_8_1","unstructured":"\u00a0"},{"key":"e_1_2_7_9_2","volume-title":"Amines: synthesis, properties and applications","author":"Lawrence S. 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