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The industrial conversion of N<jats:sub>2<\/jats:sub> into ammonia requires extremely high temperatures and pressures. Herein we report the first example of N<jats:sub>2<\/jats:sub> and O<jats:sub>2<\/jats:sub> cleavage by a uranium complex, [N(CH<jats:sub>2<\/jats:sub>CH<jats:sub>2<\/jats:sub>NP<jats:sup>i<\/jats:sup>Pr<jats:sub>2<\/jats:sub>)<jats:sub>3<\/jats:sub>U]<jats:sub>2<\/jats:sub>(TMEDA), under ambient conditions without an external reducing agent. The N<jats:sub>2<\/jats:sub> triple bond breaking implies a U<jats:sup>III<\/jats:sup>\u2013P<jats:sup>III<\/jats:sup> six\u2010electron reduction. The hydrolysis of the N<jats:sub>2<\/jats:sub> reduction product allows the formation of ammonia or nitrogen\u2010containing organic compounds. The interaction between U<jats:sup>III<\/jats:sup> and P<jats:sup>III<\/jats:sup> in this molecule allows an eight\u2010electron reduction of two O<jats:sub>2<\/jats:sub> molecules. This study establishes that the combination of uranium and a low\u2010valent nonmetal is a promising strategy to achieve a full N<jats:sub>2<\/jats:sub> and O<jats:sub>2<\/jats:sub> cleavage under ambient conditions, which may aid the design of new systems for small molecules activation.<\/jats:p>","DOI":"10.1002\/anie.202012198","type":"journal-article","created":{"date-parts":[[2020,9,25]],"date-time":"2020-09-25T15:33:45Z","timestamp":1601048025000},"page":"473-479","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":71,"title":["Facile Dinitrogen and Dioxygen Cleavage by a Uranium(III) Complex: Cooperativity Between the Non\u2010Innocent Ligand and the Uranium Center"],"prefix":"10.1002","volume":"60","author":[{"given":"Penglong","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Iskander","family":"Douair","sequence":"additional","affiliation":[{"name":"LPCNO, CNRS &amp; INSA Universit\u00e9 Paul Sabatier  135 Avenue de Rangueil 31077 Toulouse France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Zhao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuao","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Radiation Medicine and Protection School for Radiological and interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions Soochow University  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Laurent","family":"Maron","sequence":"additional","affiliation":[{"name":"LPCNO, CNRS &amp; INSA Universit\u00e9 Paul Sabatier  135 Avenue de Rangueil 31077 Toulouse France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4722-0484","authenticated-orcid":false,"given":"Congqing","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2020,10,26]]},"reference":[{"key":"e_1_2_6_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aar6611"},{"key":"e_1_2_6_2_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1073877"},{"key":"e_1_2_6_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1214025"},{"key":"e_1_2_6_4_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1206445"},{"key":"e_1_2_6_5_1","first-page":"nwaa142","author":"Lv Z.-J.","year":"2020","journal-title":"Natl. 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