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Reactions of <jats:bold>10<\/jats:bold>[Ga<jats:sub>2<\/jats:sub>Cl<jats:sub>7<\/jats:sub>] with nucleophiles (Cl<jats:sup>\u2212<\/jats:sup> or NHC) result in rare, selective P\u2013C bond cleavages, affording Ga<jats:sub>2<\/jats:sub>Cl<jats:sub>y<\/jats:sub>\u2010substituted triphosphiranes (LP<jats:sub>3<\/jats:sub>Ga<jats:sub>2<\/jats:sub>Cl<jats:sub>y<\/jats:sub>, y = \u00a05, 6) via an intramolecular ring closure mechanism. Protonation of <jats:bold>6<\/jats:bold>[GaCl<jats:sub>4<\/jats:sub>] gives rise to a similar ring closure, but without P\u2013C bond cleavage, to afford the L<jats:sub>2<\/jats:sub>P<jats:sub>3<\/jats:sub>H<jats:sup>+<\/jats:sup> salt <jats:bold>8<\/jats:bold>[OTfGaCl<jats:sub>3<\/jats:sub>]<jats:sub>2<\/jats:sub>. Additionally, the palladium complex <jats:bold>26<\/jats:bold>[GaCl<jats:sub>4<\/jats:sub>], formed through the reaction of <jats:bold>10<\/jats:bold>[Ga<jats:sub>2<\/jats:sub>Cl<jats:sub>7<\/jats:sub>] with [Pd(PPh<jats:sub>3<\/jats:sub>)<jats:sub>4<\/jats:sub>], presents a novel bicyclic P<jats:sub>3<\/jats:sub>Pd moiety (LP<jats:sub>3<\/jats:sub>Pd(PPh<jats:sub>3<\/jats:sub>)<jats:sub>2<\/jats:sub>[GaCl<jats:sub>4<\/jats:sub>]). Comprehensive DFT calculations have been conducted to elucidate the bonding situation in <jats:bold>26<\/jats:bold>[GaCl<jats:sub>4<\/jats:sub>], uncovering significant metal\u2010to\u2010ligand \u03c0\u2010back\u2010donation and a distinctive 3\u2010center\u20104\u2010electron hyperbonding phenomenon in the P\u2083Pd framework. These findings offer valuable insights into chemistry of cyclic polyphosphorus compounds and, in particular, the reactivity, structural flexibility, and the coordination properties of cationic triphosphorus species.<\/jats:p>","DOI":"10.1002\/chem.202501311","type":"journal-article","created":{"date-parts":[[2025,5,21]],"date-time":"2025-05-21T07:59:48Z","timestamp":1747814388000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Synthesis and Reactivity of Triphosphaallyl Cation Stabilized by N\u2010Heterocyclic Carbenes"],"prefix":"10.1002","volume":"31","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5079-1491","authenticated-orcid":false,"given":"Julia","family":"Fr\u00f6tschel\u2010Rittmeyer","sequence":"first","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3729-030X","authenticated-orcid":false,"given":"Felix","family":"Hennersdorf","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5886-3699","authenticated-orcid":false,"given":"Jannis","family":"Fidelius","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Chris","family":"Sala","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0956-5230","authenticated-orcid":false,"given":"Christoph","family":"Ziegler","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Regensburg  93040 Regensburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Michael","family":"Holthausen","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7965-2647","authenticated-orcid":false,"given":"Kai","family":"Schwedtmann","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4066-6483","authenticated-orcid":false,"given":"Robert","family":"Wolf","sequence":"additional","affiliation":[{"name":"Institute of Inorganic Chemistry University of Regensburg  93040 Regensburg Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7323-7816","authenticated-orcid":false,"given":"Jan J.","family":"Weigand","sequence":"additional","affiliation":[{"name":"Faculty of Chemistry and Food Chemistry Technische Universit\u00e4t Dresden  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2025,6,4]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CS00682A"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00405a054"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1160768"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja807828t"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.200902840"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2006.07.007"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja411667f"},{"key":"e_1_2_8_7_2","doi-asserted-by":"publisher","DOI":"10.1039\/c1cc13224e"},{"key":"e_1_2_8_7_3","doi-asserted-by":"publisher","DOI":"10.1021\/om4002268"},{"key":"e_1_2_8_7_4","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200902344"},{"key":"e_1_2_8_7_5","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.617"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5DT03014E"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CC08248J"},{"key":"e_1_2_8_10_1","unstructured":"a)S.Yao Tris(trimethylsilyl)silyl stabilized phosphorus and lead clusters 2005;"},{"key":"e_1_2_8_10_2","volume":"833","author":"Wiberg N.","year":"1998","journal-title":"Eur. 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