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Here we report an alternative mode of complete CO cleavage mediated by a mononuclear uranium(IV) borohydride complex supported by a double layer N\u2013P ligand at room temperature. Single\u2010crystal x\u2010ray diffraction reveals that the oxygen atom becomes bonded to both uranium and boron (U\u2013O\u2013B), while the carbon atom is inserted into a new hydrocarbyl framework, forming U\u2500C, C\u2500C, and C\u2500Si bonds. Computational studies elucidate a cooperative mechanism involving CO insertion into the U\u2013H\u2013B linkage followed by low\u2010barrier rearrangements. This work demonstrates complete CO cleavage by a mononuclear actinide complex operating through a U\u2013H\u2013B cooperative pathway, thereby establishing an alternative, nitride\u2010free route for this transformation at a single uranium center.<\/jats:p>","DOI":"10.1002\/anie.1233737","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T14:03:32Z","timestamp":1787148212000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Facile C\u2261O Triple Bond Cleavage of Carbon Monoxide by a Mononuclear Uranium Borohydride Complex"],"prefix":"10.1002","volume":"65","author":[{"given":"Yafei","family":"Li","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 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianze","family":"Xu","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 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thayalan","family":"Rajeshkumar","sequence":"additional","affiliation":[{"name":"LPCNO, CNRS &amp; 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