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Addition of tris(pentafluorophenyl)borane (BCF) to 1<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> resulted in the zwitterionic compounds 1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PHR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>)BF(C6<\/jats:sub>F5<\/jats:sub>)2<\/jats:sub> (2<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold>) through nucleophilic para<\/jats:italic> substitution of a C6<\/jats:sub>F5<\/jats:sub> ring followed by fluoride transfer to boron. Further reaction with Me2<\/jats:sub>SiHCl prompted a H\u2212F exchange yielding the zwitterionic compounds 1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PHR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>)BH(C6<\/jats:sub>F5<\/jats:sub>)2<\/jats:sub> (3<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold>). The reaction of 2<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> with one equivalent of R'MgBr (R\u2019=Me, Ph) gave the extremely water\u2010sensitive frustrated Lewis pairs 1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>)B(C6<\/jats:sub>F5<\/jats:sub>)2<\/jats:sub> (4<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold>). Hydrolysis of the B\u2212C6<\/jats:sub>F4<\/jats:sub> bond in 4<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> gave the first tertiary B<\/jats:italic>\u2010carboranyl phosphines with three distinct substituents, 1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>H) (5<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold>). Deprotonation of the zwitterionic compounds 2<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> and 3<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> formed anionic phosphines [1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>)BX(C6<\/jats:sub>F5<\/jats:sub>)2<\/jats:sub>]\u2212<\/jats:sup>[DMSOH]+<\/jats:sup> (R=Mes, X=F (6<\/jats:bold>\u2009a<\/jats:bold>), R=t<\/jats:italic>Bu, X=F (6<\/jats:bold>\u2009b<\/jats:bold>); R=Mes, X=H (7<\/jats:bold>\u2009a<\/jats:bold>), R=t<\/jats:italic>Bu, X=H (7<\/jats:bold>\u2009b<\/jats:bold>)). Reaction of 2<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> with an excess of Grignard reagents resulted in the addition of R\u2019 at the boron atom yielding the anions [1,7\u2010H2<\/jats:sub>C2<\/jats:sub>B10<\/jats:sub>H9<\/jats:sub>\u20109\u2010PR(p<\/jats:italic>\u2010C6<\/jats:sub>F4<\/jats:sub>)BR\u2019(C6<\/jats:sub>F5<\/jats:sub>)2<\/jats:sub>]\u2212<\/jats:sup> (R=Mes, R\u2019=Me (8<\/jats:bold>\u2009a<\/jats:bold>), R=t<\/jats:italic>Bu, R\u2019=Me (8<\/jats:bold>\u2009b<\/jats:bold>); R=Mes, R\u2019=Ph (9<\/jats:bold>\u2009a<\/jats:bold>), R=t<\/jats:italic>Bu, R\u2019=Ph (9<\/jats:bold>\u2009b<\/jats:bold>)) with [MgBr(Et2<\/jats:sub>O)n<\/jats:italic><\/jats:sub>]+<\/jats:sup> as counterion. The ability of the zwitterionic compounds 3<\/jats:bold>\u2009a<\/jats:bold>, b<\/jats:bold> to hydrogenate imines as well as the Br\u00f8nsted acidity of 3<\/jats:bold>\u2009a<\/jats:bold> were investigated.<\/jats:p>","DOI":"10.1002\/chem.202200531","type":"journal-article","created":{"date-parts":[[2022,4,26]],"date-time":"2022-04-26T14:11:49Z","timestamp":1650982309000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Exploring the Reactivity of B\u2010Connected Carboranylphosphines in Frustrated Lewis Pair Chemistry: A New Frame for a Classic System"],"prefix":"10.1002","volume":"28","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0490-8107","authenticated-orcid":false,"given":"Jan","family":"Schulz","sequence":"first","affiliation":[{"name":"Leipzig University, Faculty of Chemistry and Mineralogy Institute of Inorganic Chemistry Johannisallee 29 04103 Leipzig Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4222-0717","authenticated-orcid":false,"given":"Menyh\u00e1rt B.","family":"S\u00e1rosi","sequence":"additional","affiliation":[{"name":"Leipzig University, Faculty of Chemistry and Mineralogy Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry Linn\u00e9stra\u00dfe 2 04103 Leipzig Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4267-0603","authenticated-orcid":false,"given":"Evamarie","family":"Hey\u2010Hawkins","sequence":"additional","affiliation":[{"name":"Leipzig University, Faculty of Chemistry and Mineralogy Institute of Inorganic Chemistry Johannisallee 29 04103 Leipzig Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2022,5,12]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1134230"},{"key":"e_1_2_8_2_1","unstructured":"\u00a0"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b06794"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.05.007"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c10845"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200901636"},{"key":"e_1_2_8_6_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.200901636"},{"key":"e_1_2_8_7_1","unstructured":"\u00a0"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201208750"},{"key":"e_1_2_8_8_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201208750"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja401492s"},{"key":"e_1_2_8_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201503455"},{"key":"e_1_2_8_10_3","first-page":"8870","volume":"30","year":"2015","journal-title":"Angew. 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