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The boron compound FmesBCl<jats:sub>2<\/jats:sub> [Fmes: 2,4,6\u2010tris(trifluoromethyl)phenyl] reacted with three molar equivalents of the lithio\u2010acetylene reagent Li\u2010C\u2261C\u2010Fmxyl [Fmxyl: 3,5\u2010bis(trifluoromethyl)phenyl]. Subsequent crystallization from benzene gave the [bis(\u03b7<jats:sup>6<\/jats:sup>\u2010benzene)Li]<jats:sup>+<\/jats:sup> cation with the [{FmesB(\u2010C\u2261C\u2010Fmxyl)<jats:sub>3<\/jats:sub>}<jats:sub>2<\/jats:sub>Li]<jats:sup>\u2212<\/jats:sup> anion. This parent [(arene)<jats:sub>2<\/jats:sub>Li]<jats:sup>+<\/jats:sup> cation shows an eclipsed arrangement of the pair of benzene ligands at the central lithium cation with uniform carbon\u2010lithium bond lengths. The corresponding [(\u03b7<jats:sup>6<\/jats:sup>\u2010toluene)<jats:sub>2<\/jats:sub>Li]<jats:sup>+<\/jats:sup> and [(\u03b7<jats:sup>6<\/jats:sup>\u2010durene)<jats:sub>2<\/jats:sub>Li]<jats:sup>+<\/jats:sup> containing salts were similarly prepared. The bis(arene)lithium cations were characterized by X\u2010ray diffraction, by solid\u2010state <jats:sup>7<\/jats:sup>Li MAS NMR spectroscopy and their bonding features were analyzed by DFT calculations.<\/jats:p>","DOI":"10.1002\/anie.202108376","type":"journal-article","created":{"date-parts":[[2021,8,7]],"date-time":"2021-08-07T14:31:55Z","timestamp":1628346715000},"page":"22879-22884","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["The Bis(\u03b7<sup>6<\/sup>\u2010benzene)lithium Cation: A Fundamental Main\u2010Group Organometallic Species"],"prefix":"10.1002","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-3333-3082","authenticated-orcid":false,"given":"Xiaoming","family":"Jie","sequence":"first","affiliation":[{"name":"Organisch-Chemisches Institut Westf\u00e4lische Wilhelms-Universit\u00e4t M\u00fcnster  Corrensstra\u00dfe 40 48149 M\u00fcnster 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