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While the phosphine\u2010silylene\u2010substituted dicarborane <jats:bold>1<\/jats:bold>, CB\u2010<jats:bold>SiP<\/jats:bold> (CB=<jats:italic>ortho<\/jats:italic>\u2010C,C\u2032\u2010C<jats:sub>2<\/jats:sub>B<jats:sub>10<\/jats:sub>H<jats:sub>10<\/jats:sub>, <jats:bold>Si<\/jats:bold>=PhC(tBuN)<jats:sub>2<\/jats:sub>Si, <jats:bold>P<\/jats:bold>=P[N(tBu)CH<jats:sub>2<\/jats:sub>]<jats:sub>2<\/jats:sub>), activates white phosphorus in a 2\u2009:\u20091 molar ratio to yield the P<jats:sub>5<\/jats:sub>\u2010chain containing species <jats:bold>2<\/jats:bold>, the analogous bis(silylene)\u2010substituted compound <jats:bold>3<\/jats:bold>, CB\u2010<jats:bold>Si<jats:sub>2<\/jats:sub><\/jats:bold><jats:sub>,<\/jats:sub> reacts with P<jats:sub>4<\/jats:sub> in the molar ratio of 2\u2009:\u20091 to furnish the first isolable 1,3\u2010diphospha\u20102,4\u2010disilabutadiene (Si=P\u2212Si=P\u2010containing) compound <jats:bold>4<\/jats:bold>. For the latter reaction, two intermediates having a CB\u2010Si<jats:sub>2<\/jats:sub>P<jats:sub>4<\/jats:sub> and CB\u2010Si<jats:sub>2<\/jats:sub>P<jats:sub>2<\/jats:sub> core could be observed by multinuclear NMR spectroscopy. The compounds <jats:bold>2<\/jats:bold> and <jats:bold>4<\/jats:bold> were characterized including single\u2010crystal X\u2010ray diffraction analyses. Their electronic structures and mechanisms were investigated by density functional theory calculations.<\/jats:p>","DOI":"10.1002\/anie.202205358","type":"journal-article","created":{"date-parts":[[2022,5,3]],"date-time":"2022-05-03T05:58:02Z","timestamp":1651557482000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Unexpected White Phosphorus (P<sub>4<\/sub>) Activation Modes with Silylene\u2010Substituted <i>o<\/i>\u2010Carboranes and Access to an Isolable 1,3\u2010Diphospha\u20102,4\u2010disilabutadiene"],"prefix":"10.1002","volume":"61","author":[{"given":"Yun","family":"Xiong","sequence":"first","affiliation":[{"name":"Department of Chemistry: Metalorganics and Inorganic Materials Technische Universit\u00e4t Berlin  Strasse des 17. Juni 135, Sekr. C2 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shicheng","family":"Dong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surface and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shenglai","family":"Yao","sequence":"additional","affiliation":[{"name":"Department of Chemistry: Metalorganics and Inorganic Materials Technische Universit\u00e4t Berlin  Strasse des 17. Juni 135, Sekr. C2 10623 Berlin Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Zhu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surface and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9873-4103","authenticated-orcid":false,"given":"Matthias","family":"Driess","sequence":"additional","affiliation":[{"name":"Department of Chemistry: Metalorganics and Inorganic Materials Technische Universit\u00e4t Berlin  Strasse des 17. Juni 135, Sekr. 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