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Upon reaction with [MnBr(CO)<jats:sub>5<\/jats:sub>], an octahedral 18\u2010electron complex [Mn(CO)<jats:sub>3<\/jats:sub>(<jats:bold>L<\/jats:bold>)]Br (<jats:bold>1<\/jats:bold>) is obtained in which <jats:bold>L<\/jats:bold> adopts a facial arrangement. After deprotonation of the NH group in the cationic complex unit, a neutral Mn(I) amido complex [Mn(CO)<jats:sub>2<\/jats:sub>(<jats:bold>L<\/jats:bold>\u2010<jats:bold>H<\/jats:bold>)] (<jats:bold>2<\/jats:bold>) is formed under loss of CO. Rearrangement of <jats:bold>L<\/jats:bold>\u2010<jats:bold>H<\/jats:bold> leads to a trigonal bipyramidal structure in which the P and N donor centers are in <jats:italic>trans<\/jats:italic> position. Further deprotonation of <jats:bold>2<\/jats:bold> results in a dep\u2010blue anionic complex fragment [Mn(CO)<jats:sub>2<\/jats:sub>(<jats:bold>L<\/jats:bold>\u2010<jats:bold>2H<\/jats:bold>)]<jats:sup>\u2212<\/jats:sup> (<jats:bold>3<\/jats:bold>). DFT calculations and a QTAIM analysis show that the amido complex\u2005<jats:bold>2<\/jats:bold> contains a Mn\u2010N bond with partial double bond character and <jats:bold>3<\/jats:bold> an aromatic MnN<jats:sub>2<\/jats:sub>C<jats:sub>2<\/jats:sub> ring. The anion [Mn(CO)<jats:sub>2<\/jats:sub>(<jats:bold>L<\/jats:bold>\u2010<jats:bold>2H<\/jats:bold>)]<jats:sup>\u2212<\/jats:sup> reacts with Ph<jats:sub>2<\/jats:sub>PH to give a phosphido complex, which serves as phosphide transfer reagent to activated olefins. But the catalytic activity is low. However, the neutral amido complex\u2005<jats:bold>2<\/jats:bold> is an excellent catalyst and with loadings as low as 0.04\u2005mol\u2009%, turn over frequencies of &gt;40\u2019000\u2005h<jats:sup>\u22121<\/jats:sup> can be achieved. Furthermore, secondary and primary alkyl phosphines as well as PH<jats:sub>3<\/jats:sub> can be added in a catalytic hydrophosphination reaction to a wide range of activated olefins such as \u03b1,\u03b2\u2010unsaturated aldehydes, ketones, esters, and nitriles. But also, vinyl pyridine and some styrene derivatives are converted into the corresponding phosphanes.<\/jats:p>","DOI":"10.1002\/chem.202303848","type":"journal-article","created":{"date-parts":[[2024,2,7]],"date-time":"2024-02-07T02:16:29Z","timestamp":1707272189000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["A Simple Manganese(I) Catalyst for the Efficient and Selective Hydrophosphination of Olefins with PH<sub>3<\/sub>, Primary, and Secondary Phosphanes"],"prefix":"10.1002","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3945-3210","authenticated-orcid":false,"given":"Aabid A.","family":"Wani","sequence":"first","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Z\u00fcrich Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1171-6886","authenticated-orcid":false,"given":"Juan Jos\u00e9 Gamboa","family":"Carballo","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Applied Biosciences ETH  Z\u00fcrich Vladimir-Prelog-Weg 1 CH-8093 Zurich Switzerland"},{"name":"Higher Institute of Technologies and Applied Sciences (InSTEC) University of Havana  Ave. S. 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