Crossing Organolithium Compounds with Organolithium Compounds: Molecular Squares and a Cage‐Encapsulating Reaction

Triple-crossed: An extraordinary crossing reaction involving three popular utility organolithium reagents nBuLi, LiTMP (TMP=2,2,6,6-tetramethylpiperidide), and LiC5H5 leads to the unexpected deprotonation of C5H5− anions to C5H42− dianions, which was manifested through the trapping of the hexameric nBuLi cage by a [{Li(μ-TMP)Li(μ-C5H5)}4] molecular square ring (see picture).