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DFT calculations revealed that the preferred reaction mechanism involves the unsaturated 16\u2010e mangana\u2010substituted phosphonium ylide complex fac\u2010[Mn(CO)<jats:sub>3<\/jats:sub>(\u03ba<jats:sup>2<\/jats:sup>P,C\u2010Ph<jats:sub>2<\/jats:sub>P=CHNHC)] (<jats:bold>6\u2009b<\/jats:bold>) as key intermediate able to activate H<jats:sub>2<\/jats:sub> via a non\u2010classical mode of metal\u2010ligand cooperation implying a formal \u03bb<jats:sup>5<\/jats:sup>\u2010P\u2013\u03bb<jats:sup>3<\/jats:sup>\u2010P phosphorus valence change. Complex <jats:bold>2<\/jats:bold> is shown to be one of the most efficient pre\u2010catalysts for ketone hydrogenation in the Mn<jats:sup>I<\/jats:sup> series reported to date (TON up to 6200).<\/jats:p>","DOI":"10.1002\/anie.201901169","type":"journal-article","created":{"date-parts":[[2019,3,12]],"date-time":"2019-03-12T10:14:25Z","timestamp":1552385665000},"page":"6727-6731","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":105,"title":["Phosphine\u2010NHC Manganese Hydrogenation Catalyst Exhibiting a Non\u2010Classical Metal\u2010Ligand Cooperative H<sub>2<\/sub> Activation Mode"],"prefix":"10.1002","volume":"58","author":[{"given":"Ruqaya","family":"Buhaibeh","sequence":"first","affiliation":[{"name":"LCC-CNRS Universit\u00e9 de Toulouse, CNRS UPS  205 route de Narbonne 31077 Toulouse Cedex 4 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7963-2806","authenticated-orcid":false,"given":"Oleg A.","family":"Filippov","sequence":"additional","affiliation":[{"name":"A. 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