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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).
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