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At first, the unprecedented aluminium(III) iodide precursors [Si<jats:sup>II<\/jats:sup>(Xant)Si<jats:sup>II<\/jats:sup>]AlI<jats:sub>2<\/jats:sub><jats:sup>+<\/jats:sup> I<jats:sup>\u2212<\/jats:sup> <jats:bold>1<\/jats:bold> and [Si<jats:sup>II<\/jats:sup>(N<jats:sub>Acrid<\/jats:sub>)Si<jats:sup>II<\/jats:sup>)]AlI<jats:sub>2<\/jats:sub> <jats:bold>2<\/jats:bold> were synthesized using AlI<jats:sub>3<\/jats:sub> and [Si<jats:sup>II<\/jats:sup>(Xant)Si<jats:sup>II<\/jats:sup>] or [Si<jats:sup>II<\/jats:sup>(N<jats:sub>Acrid<\/jats:sub>)Si<jats:sup>II<\/jats:sup>)]Li(OEt<jats:sub>2<\/jats:sub>)], respectively, and structurally characterized. While reduction of <jats:bold>1<\/jats:bold> with KC<jats:sub>8<\/jats:sub> led merely to unidentified products, the dehalogenation of <jats:bold>2<\/jats:bold> afforded the dimer of the desired {[Si<jats:sup>II<\/jats:sup>(N<jats:sub>Acrid<\/jats:sub>)Si<jats:sup>II<\/jats:sup>)]Al:} aluminylene with a four\u2010membered Si<jats:sup>IV<\/jats:sup><jats:sub>2<\/jats:sub>Al<jats:sup>III<\/jats:sup><jats:sub>2<\/jats:sub> ring. Remarkably, the proposed aluminylene intermediates [Si<jats:sup>II<\/jats:sup>(Xant)Si<jats:sup>II<\/jats:sup>]Al<jats:sup>I<\/jats:sup>I and {[Si<jats:sup>II<\/jats:sup>(N<jats:sub>Acrid<\/jats:sub>)Si<jats:sup>II<\/jats:sup>)]Al:} could be produced through reaction of <jats:bold>1<\/jats:bold> and <jats:bold>2<\/jats:bold> with Collman's reagent, K<jats:sub>2<\/jats:sub>Fe(CO)<jats:sub>4<\/jats:sub>, and trapped as Al<jats:sup>I<\/jats:sup>:\u2192Fe(CO)<jats:sub>4<\/jats:sub> complexes <jats:bold>5<\/jats:bold> and <jats:bold>6<\/jats:bold>, respectively. While <jats:bold>6<\/jats:bold> is stable in solution, <jats:bold>5<\/jats:bold> loses one CO ligand in solution to afford the silylene\u2010 and aluminylene\u2010coordinated iron(0) complex <jats:bold>7<\/jats:bold> from an intramolecular substitution reaction. The electronic structures of the novel compounds were investigated by Density Functional Theory calculations.<\/jats:p>","DOI":"10.1002\/anie.202410790","type":"journal-article","created":{"date-parts":[[2024,7,18]],"date-time":"2024-07-18T18:01:05Z","timestamp":1721325665000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Bis\u2010Silylene\u2010Supported Aluminium Atoms with Aluminylene and Alane Character"],"prefix":"10.1002","author":[{"given":"Artemis","family":"Saddington","sequence":"first","affiliation":[{"name":"Department of Chemistry: Metalorganics and Inorganic Materials Technische Universit\u00e4t Berlin  Strasse des 17.\u2005Juni 115, Sekr. 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