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Our observations are consistent with the formation of a transient phosphanyl\u2010phosphaalumene at low temperatures (\u221270\u2009\u00b0C), however this species was found to readily undergo intramolecular C\u2212H activation of the \u03b2\u2010diketiminato ligand upon warming to room temperature. The reactivity of the transient complex toward small molecules including dihydrogen, carbon dioxide, phosphaketenes, amines and silanes could be explored at low temperatures, showcasing that the target compound can react as both a frustrated Lewis pair (<jats:italic>via<\/jats:italic> the pendant phosphanyl moiety) or in hydroelementation reactions of the Al=P bond. The elusive target molecule could be trapped by addition of a Lewis base (tetrahydrofuran) affording an isolable molecular species that reacts in an analogous fashion to the base\u2010free compound.<\/jats:p>","DOI":"10.1002\/chem.202401326","type":"journal-article","created":{"date-parts":[[2024,4,12]],"date-time":"2024-04-12T13:09:52Z","timestamp":1712927392000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Trapping an Elusive Phosphanyl\u2010Phosphaalumene"],"prefix":"10.1002","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2445-6366","authenticated-orcid":false,"given":"Lilian S.","family":"Szych","sequence":"first","affiliation":[{"name":"Department of Chemistry University of Oxford Chemistry Research Laboratory  12 Mansfield Road OX1\u20093TA Oxford U.K."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-2909-7043","authenticated-orcid":false,"given":"Lars","family":"Denker","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Oxford Chemistry Research Laboratory  12 Mansfield Road OX1\u20093TA Oxford U.K."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Joey","family":"Feld","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Oxford Chemistry Research Laboratory  12 Mansfield Road OX1\u20093TA Oxford U.K."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7311-1663","authenticated-orcid":false,"given":"Jose M.","family":"Goicoechea","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indiana University  800 E. 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